Measuring true electromechanical strain of electroactive thermoplastic elastomer gels using synchrotron SAXS

The true electric actuation thickness strain of poly (styrene‐b‐ethylbutylene‐b‐styrene) (SEBS) gel was measured using an in situ synchrotron SAXS. The thermoplastic elastomer SEBS gel was microphase‐separated to form a disordered styrene micelle nanostructure in an oil‐swollen ethylbutylene matrix. The SEBS gel showed reversible cyclic load–unload compression behavior without permanent residual strain. The electromechanical strain of the SEBS gel with carbon paste electrodes could be evaluated by means of a nanostructure dimensional change traced by using the in situ synchrotron SAXS during actuation. The strain measured with SAXS was compared with the strain measured using conventional laser displacement sensor systems. The optical laser sensor method was likely to overestimate the thickness strain due to the bending movement of the dielectric elastomer. To our knowledge, the thickness strain value measured by the synchrotron SAXS is the closest to the true strain ever measured in the field of dielectric elastomer studies, because the nanostructure dimensional change depends on the thickness dimension change, not on the translational movement like the bending motion. © 2010 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys, 2010     

Thermal actuation of hydrogels from PNIPAm,alginate, and carbon nanofibres

Composite ionic‐covalent entanglement (ICE) hydrogel networks were prepared from poly(N‐isopropylacrylamide), alginate, and carbon nanofibres. An optimised triple network hydrogel with 86% water content exhibited a compressive strength of 3.0 ± 0.1 MPa and 66 ± 13 mS/cm electrical conductivity. Thermal actuation was shown to have a shorter response time for gels containing nanofibres, compared to those which did not and hydrogel samples more than halved in volume within 1 minute when placed in a 60 °C water bath. Controlled dye release was demonstrated as a potential application and used to further quantify thermal actuation over short times. Joule heating techniques were used to electronically actuate the hydrogel samples, removing the traditional requirements for immersion in a temperature controlled liquid. It is expected that devices based on these materials will find potential applications in soft robotics and micro fluidics. © 2017 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2018 , 56, 46–52     

A fully coupled thermo‐viscoelastic finite element model for self‐folding shape memory polymer sheets

The thermo‐mechanical response of heat activated shape memory polymers (SMPs) has been investigated using a thermo‐viscoelastic finite element analysis that accounts for external and internal heat sources. SMPs can be thermally stimulated by external heat sources, such as temperature and surface heat flux, or from internal viscous heating. Viscous heating can significantly affect the response of SMP sheets by increasing the temperature during pre‐strain, which accelerates stress relaxation. This stress relaxation results in a slower shrinking rate when the SMP is reheated. Viscous heating also causes an increase in temperatures during unconstrained recovery. The predicted results elucidate how the coupled thermo‐mechanical loading conditions affect folding and unfolding of SMP sheets in response to localized heating in a hinged region. A parametric study of sheet thickness, hinge width, degree of pre‐strain, and hinge surface temperature is also conducted. The validated results can provide guidelines for the design of functional, self‐folding structures. © 2017 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2017 , 55, 1207–1219     

On the relevance of the 8‐chain model and the full‐network model for the deformation and failure of networks formed through photopolymerization of multifunctional monomers

Crosslinked networks were synthesized by copolymerization of mono‐functional tert‐butyl acrylate (tBA) with diethyleneglycol dimethacrylate (DEGDMA) or polyethylene glycol dimethacrylates (PEGDMA). By varying the chain length and concentration of the difunctional PEGDMA, we obtained tBA‐PEGDMA copolymer networks while by varying the concentration of difunctional DEGDMA, we obtained tBA‐DEGDMA crosslinked networks. The various materials were submitted to large deformations through uniaxial tension tests. For moderate weight percent of crosslinking agent, up to 20%, the networks showed standard S‐shape stress–strain curves, characteristic of rubber‐like elasticity. Two macromolecular models, the 8‐chain model and the full‐network model, were applied to fit the uniaxial tensile response of the materials. Both models provide good representations of the overall uniaxial stress–strain response of each material. After fitting to stress–strain data, the network models were employed to predict the shear modulus and the elongation at break. Neither the 8‐chain nor the full network model were capable of predicting the failure strain or shear modulus, indicating these models are best used to describe stress–strain relations rather than predict mechanical properties for the network polymers considered here. © 2008 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys 46: 1226–1234, 2008     

pH/temperature double responsive behaviors and mechanical strength of laponite‐crosslinked poly(DEA‐co‐DMAEMA) nanocomposite hydrogels

A nanocomposite (NC) hydrogel crosslinked by inorganic Laponite XLG was successfully synthesized via in situ free radical polymerization of monomers N,N‐diethylacrylamide and (2‐dimethylamino) ethyl methacrylate (DMAEMA). Polymerization was carried out at room temperature due to the accelerating effect of DMAEMA. The as‐prepared hydrogels displayed controlled transformation in optical transmittance and volume in response to small diversification of environmental factors, such as temperature and pH. The compressive strength of swollen D_6:1G₆ hydrogels was as high as 2219 kPa while compressive strain was 95%. Cyclic compression measurement exhibited good elastic properties of NC hydrogels. This work provides a facile method for fabricating stimuli‐responsive hydrogels with superior mechanical property. © 2015 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2015 , 53, 876–884     

Zr(IV)‐Crosslinked Polyacrylamide/Polyanionic Cellulose Composite Hydrogels with High Strength and Unique Acid Resistance

Recently, metal coordination has been widely utilized to fabricate high‐performance hydrogels, but conventional metal‐based hydrogels face some drawbacks, such as staining or acid lability. In the present study, a novel kind of colorless Zr(IV)‐crosslinked polyacrylamide/polyanionic cellulose (PAM/PAC) composite hydrogel with unique acid resistance was constructed via acrylamide polymerization in a PAC solution, followed by posttreatment in a zirconium oxychloride (ZrOCl₂) solution. The prepared gels were characterized in terms of Fourier transform infrared spectroscopy, scanning electron microscopy, and tensile and compressive mechanics, as well as acid resistance. Inside the gels, the synergistic action of hydrogen bonding and Zr(IV) coordination is responsible for their improved mechanical properties and good energy dissipation ability. One hydrogel with nearly 90 wt % of water content can sustain approximately 5 MPa of compression stress at 90% strain without damage. Both microscopic network structures and macroscopic mechanics demonstrate facile adjustability via changing the PAC dosages in polymerization and/or ZrOCl₂ concentrations in posttreatment. Moreover, the gels present unexpected acid resistance due to the strong Zr(IV) coordination with PAC, demonstrating their potential application as hydrogel electrolytes in supercapacitors. The current work provides a new approach to fabricate metal coordination‐based high strength, colorless hydrogels with acid resistance. © 2019 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2019 , 57, 981–991     

Mechanical recoverability and damage process of ionic‐covalent PAAm‐alginate hybrid hydrogels

Hydrogels consisting of interpenetrating networks of ionically and covalently crosslinked polymers showed high toughness and mechanical recoverability as a result of the dissociation and re‐formation of ionic crosslinks. The present investigation aimed to provide a quantitative study on the mechanical recoverability and damage process of an example hybrid gel of calcium crosslinked alginate and covalently crosslinked polyacrylamide. Three series of load/unload tests were performed sequentially with the mechanical properties of the gel fully retrieved between the 2nd and 3rd load/unload series while only the partial recovery of mechanical properties was evident from the 1st to 2nd series. The load/unload curves in the three series were modeled by existing mechanical models, and the fitted model parameters clearly demonstrate a damage process for the hybrid gel. When a hybrid gel was deformed above its historic maximum strain, the shortest alginate chains were fully‐stretched, pulling apart the weak ionic crosslinks and dissipating fracture energy. Consequently, the strand density of the intact gel network was reduced and the contour length of the remaining next‐shortest load‐bearing alginate chains became longer. A log‐normal distribution was used to describe the probability distribution for the strand fracture and also to describe the strand length distribution of the ionic network. © 2015 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2016 , 54, 53–63     

Structural rearrangement and stiffening of hydrophobically modified supramolecular hydrogels during thermal annealing

Dynamic crosslinks formed by thermoreversible associations provide an energy dissipation mechanism to toughen hydrogels. However, the details of the organization of these crosslinks impact the hydrogel properties through constraints on the network chain conformation. The physical crosslinks generated by hydrophobic association of the 2‐(N‐ethylperfluorooctane‐sulfonamido)ethyl methacrylate (FOSM) groups in a random copolymer of N,N‐dimethylacrylamide (DMA) and FOSM provide a simple system to investigate how the hydrogel structure (as determined from small angle neutron scattering impacts the mechanical properties of the hydrogel. The initial hydration of the copolymer at 25 °C leads to a kinetically trapped structure with large‐scale heterogeneities. Heating the hydrogel at 60 °C, which is above the glass transition temperature for the FOSM domains, allows the hydrogel structure to rearrange to reduce the density of network defects and the structural heterogeneities. That effectively increases the crosslink density of the network, which stiffens the hydrogel and decreases the swelling at equilibrium at 25 °C. The processing history determines how the hydrophobes aggregate to form the physically crosslinked network, whose structure defines the mechanical properties of these hydrogels. © 2017 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2017 , 55, 1036–1044     

Fast and excellent healing of hydroxypropyl guar gum/poly(N,N‐dimethyl acrylamide) hydrogels

In this article, a fast and high efficient healing hydroxypropyl guar gum (HPG)/poly(N,N‐dimethyl acrylamide) (PDMA) hydrogel is prepared by a facile synthesis method. HPG networks are formed through hydrogen‐bond interaction between the hydroxyl groups in the HPG chains, and PDMA networks are self‐crosslinked without any chemical crosslinker. The cut hydrogel could heal when nanosilica solution is chosen as the connector that is related to the adsorption of polymer to the surface of nanosilica. The fracture stress of the HPG/PDMA gels presents a fast and almost full recovery within a short time (1 min), while the recovery of fracture strain and elastic modulus is related to time in 2 h. The healing efficiency of HPG/PDMA gel is investigated as a function of healing time, HPG content, and N,N‐dimethyl acrylamide content. The microscopic healing process and healing mechanism are also discussed. © 2017 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2018 , 56, 239–247     

Transient bioelectronics: Electronic properties of silver microparticle‐based circuits on polymeric substrates subjected to mechanical load

Transient soft bioelectronics are capable of forming conformal contacts with curvilinear surfaces of biological host tissues and organs. Such systems are often subject to continuous static and dynamic loads from the biological host. In this article, we present investigation of electronic attributes of transient soft bioelectronic circuits subjected to mechanical force and influence of substrate's transiency on the transiency of the whole device; also, characterize and quantify loss of functionality in triggered devices. Variations in the electrical conductivity of circuits as a function of applied mechanical load was used as a means to deduce electronic characteristics under stress. The experimental results suggest that there exists a correlation between electronic properties of circuits and applied mechanical strain; no clear correlation was, however, observed between electronic properties of circuits and frequency of the applied dynamic load. Control over transiency rate of identical circuits utilizing the transiency characteristics of the poly(vinyl alcohol)l‐based substrates is also studied and demonstrated. © 2015 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2015 , 53, 1603–1610     

Synthesizing a new dielectric elastomer exhibiting large actuation strain and suppressed electromechanical instability without prestretching

Prestrain provides high actuation performance in dielectric elastomers (DEs) but increases the bulk, mass, and fatigue of the resulting actuators. Based on our experiments on prestrain‐locked interpenetrating polymer films and the model developed by Zhao and Suo, materials with a certain stress–strain relationship should be capable of high strain without prestrain by suppressing electromechanical instability (EMI). Here, we report the synthesis of an acrylic elastomer capable of achieving high actuation performance without prestrain. DE films were directly fabricated by ultraviolet curing of precursors comprising a mixture of acrylate comonomers. Varying the amount of crosslinker comonomer in the precursor allowed us to tune the stress–strain relationship and completely suppress EMI while maintaining high strain performance. Addition of plasticizing agents increased strain sensitivity. The result is a new DE, synthesized from scratch, capable of high actuation strain (>100%), high energy density (>1 J g^?1), and good temperature and frequency response without requiring prestretching. The material can be fabricated using conventional coating techniques and the process can allow for high volume throughput of stacked DE actuators. © 2012 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys, 2013     

Influence of Plasticizers on the Electromechanical Behavior of a P(VDF‐TrFE‐CTFE) Terpolymer: Toward a High Performance of Electrostrictive Blends

This work aims at providing a complete analysis of the effect of plasticizers on the electrostrictive terpolymer performance. To achieve this, several plasticizing agents such as 2‐ethylhexyl phtalate (DEHP), diisononyl phtalate (DINP), and palamoll 652 have been incorporated in the polymer matrix. Experimental results demonstrate that the proposed novel materials exhibited excellent electromechanical enhancement in terms of transverse strain and mechanical energy density under a moderate electric field, which is definitively critical in recent microscale actuation. Another objective of this article was to explore material characteristics as a function of the DINP content, and it was found that the plasticizer weigh fraction was the key parameter determining performance of the modified fluorinate terpolymer blends. Accordingly, it was revealed that high performance flexible actuators can be achieved merely by employing a simple and cheap plasticizer, thus making it possible to overcome the current technological barrier of conventional electroactive polymers that suffer from the high applied electric field usually required to reach sufficient strain. © 2016 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2017 , 55, 355–369     

Investigation on the mechanical behavior of poly(2‐hydroxyethyl methacrylate) hydrogel membrane under compression in the assembly process of microfluidic system

A microfluidic system with an inserted membrane assembled using mechanical fastening process is described. The membrane is made of a biocompatible water swollen poly(2‐hydroxyethyl methacrylate) (PHEMA) hydrogel thin film as a sealing component. The hyperelastic characteristics of PHEMA membrane under the compression during fastening are investigated through numerical simulations, including strain and Von Mises stress distribution, and potential fracture in correlation with the microchannel's geometry and dimensions. To validate the modeling, the experiments have also been conducted to visualize the deformation induced in membrane and internal stress distribution using 3D optical measuring system. The results from this study have revealed the implications in connection with the mechanical behavior of the PHEMA membranes in the assembly of microfluidic system through mechanical fastening technique. This will ultimately assist to produce a guideline for the optimum design of microchannels in the uses of PHEMA membranes and associated assembly process. © 2014 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2014 , 52, 485–495     

A novel sodium carboxymethylcellulose/poly(N‐isopropylacrylamide)/Clay semi‐IPN nanocomposite hydrogel with improved response rate and mechanical properties

A novel semi‐IPN nanocomposite hydrogel (CMC/PNIPA/Clay hydrogel) based on linear sodium carboxymethylcellulose (CMC) and poly(N‐isopropylacrylamide) (PNIPA) crosslinked by inorganic clay was prepared. The structure and morphology of these hydrogels were investigated and their swelling and deswelling kinetics were studied in detail. TEM images showed that the clay was substantially exfoliated to form nano‐dimension platelets dispersed homogeneously in the hydrogels and acted as a multifunctional crosslinker. The CMC/PNIPA/Clay hydrogels swell faster than the corresponding PNIPA/Clay hydrogels at pH 7.4, whereas they swell slower than the PNIPA/Clay hydrogels at pH 1.2. The CMC/PNIPA/Clay nanocomposite hydrogels showed much higher deswelling rates, which was ascribed to more passway formed in these hydrogels for water to diffuse in and out. The deswelling process of the hydrogels could be approximately described by the first‐order kinetic equation and the deswelling rate decreased with increasing clay content. The mechanical properties of the CMC/PNIPA/Clay nanocomposite hydrogels were analyzed based on the theory of rubber elasticity. It was found that with increasing clay content, the effective crosslink chain density, v_e, increased whereas the molecular weight of the chains between crosslinks M_c decreased. © 2008 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys 46: 1546–1555, 2008     

Irreversible temperature‐responsive formation of high‐strength hydrogel from an enantiomeric mixture of starburst triblock copolymers consisting of 8‐arm PEG and PLLA or PDLA

Starburst triblock copolymers consisting of 8‐arm poly(ethylene glycol) (8‐arm PEG) and biodegradable poly(L ‐lactide) (PLLA) or its enantiomer poly(D ‐lactide) (PDLA), 8‐arm PEG‐b‐PLLA‐b‐PEG ( Stri‐L ), and 8‐arm PEG‐b‐PDLA‐b‐PEG ( Stri‐D ) were synthesized. An aqueous solution of a 1:1 mixture ( Stri‐Mix ) of Stri‐L and Stri‐D assumed a sol state at room temperature, but instantaneously formed a physically crosslinked hydrogel in response to increasing temperature. The resulting hydrogel exhibited a high‐storage modulus (9.8 kPa) at 37 °C. Interestingly, once formed at the transition temperature, the hydrogel was stable even after cooling below the transition temperature. The hydrogel formation process was irreversible because of the formation of stable stereocomplexes. In aqueous solution, gradual hydrolytic erosion was observed because of degradation of the hydrogel. The combination of rapid temperature‐triggered irreversible hydrogel formation, high‐mechanical strength, and degradation behavior render this polymer mixture system suitable for use in injectable biomedical materials, for example, as a drug delivery system for bioactive reagents or a biodegradable scaffold for tissue engineering. © 2008 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem 46: 6317–6332, 2008     

Frontal polymerization for smart intrinsic self‐healing hydrogels and its integration with microfluidics

Frontal polymerization (FP) is applied for the synthesis of β‐cyclodextrin/poly(vinylimidazole‐co‐N‐vinylcaprolactam‐co‐acrylic acid) (β‐CD/P(VI‐co‐NVCL‐co‐AA)) copolymers. The dependence of frontal velocity and temperature on the initiator and cross‐linker are discussed. The synthesized copolymers have been characterized by Fourier transform infrared (FTIR), thermogravimetric analysis (TGA), and scanning electron microscopy (SEM). The thermo‐pH dual‐stimuli responsive behavior of the hydrogel is determined by swelling measurement at different temperatures and pH values. Besides, the hydrogels show intrinsic self‐healing behavior and their healing efficiency is determined by the mechanical tests. Interestingly, we integrate FP with microfluidic technology, which may realize the execution of FP under continuous condition. Such simple microfluidics‐FP integrated approach has both methodological and practical value for the synthesis of functional materials. This paper mainly presents the synthesis and characterization of β‐cyclodextrin/poly(vinylimidazole‐co‐N‐vinylcaprolactam‐co‐acrylic acid) (β‐CD/P(VI‐co‐NVCL‐co‐AA)) copolymers by using thermal frontal polymerization (TFP). Hydrogels were found to be self‐healing with good mechanical performance and show dual thermo‐pH responsive behavior. Low‐cost, energy‐saving and efficient method of thermal frontal polymerization process was integrated with microfluidics technology to prepare supraball hydrogel. © 2018 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2018 , 56, 1412–1423     

Structural origin for the strain rate dependence of mechanical response of fluoroelastomer F2314

The structural evolution of fluoroelastomer F2314 is studied during uniaxial tensile in a large strain rate range (0.1–150 s^?1) with the combination of a homemade high‐speed stretching device and in situ small‐ and wide‐angle X‐ray scattering techniques. Based on the mechanical behaviors and structural evolutions, three strain rate regions (I–III) are defined. The microphase‐separated structure plays an important role in the mechanical response of F2314. In Region I, deformation of soft domains is the main process before yielding, accompanied by the destruction of lamellar crystals in hard domains. In the stress plateau zone, deformation of hard domains is confirmed as the primary mechanism of energy dissipation. With the orientation parameter of the amorphous phase reaching a critical value, strain hardening is triggered. Recrystallization also takes place in strain hardening zone. In Region II, due to the mismatch between the mobility of molecular chains in hard domains and the acting time of stress, large deformation of hard domains is more and more difficult to occur with the disappearance of recrystallization. In Region III, as almost all molecular chains have no time to adjust or relax to fit the stress field, the sample presents a brittle fracture. © 2019 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2019 , 57, 607–620     

Mechanically tough and recoverable hydrogels via dual physical crosslinkings

Development of functional tough hydrogels with new network structures and energy dissipation mechanisms has great promise for many applications. Here, a new type of physical hydrogel crosslinked by hydrophobic association and hydrogen bonds was synthesized by a facile micellar copolymerization of hydrophobic methyl acrylate (MA) monomers and hydrophilic N-hydroxyethyl acrylamide (HEAA) monomers in the presence of Tween80 micelles. Strong hydrophobic association between inner MA and Tween80 and hydrogen bonds between external polyHEAA and Tween80 provide two distinct crosslinkers to construct mechanically tough and recoverable network. Mechanical properties of polyHEAA-MA@Tween80 hydrogels strongly depended on network components (HEAA, MA; Tween80 concentrations). At optimal conditions, the hydrogels can achieve fracture stress of 700 kPa, fracture strain of 1687 mm/mm, elastic modulus of 195 kPa, and tearing energy of 1598 J/m². Due to the reversible nature of physical interactions, polyHEAA-MA@Tween80 hydrogels can achieve fast stiffness/toughness recovery of 60%/33% without any external stimuli and resting time at room temperature. This work demonstrates a new design strategy to fabricate a new a single-network hydrogel with high mechanical and self-recovery properties by incorporating both hydrophobic association and hydrogen bonds in the network, which may provide alternative viewpoint for the design of multifunctional tough hydrogels. © 2018 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2018 , 56, 1294–1305     

Mechanical properties of hard–soft block copolymers calculated from coarse-grained molecular dynamics models

To relate the mechanical responses of hard–soft copolymer systems with their microstructures, a coarse-grained molecular dynamics approach is employed, and mechanical properties of both hard and soft domains are calculated. We first investigate the enhancement mechanism of hard domains under tensile and shear loading conditions with pressure. The energy factor that denotes the interaction between hard beads dominates the microphase separation and morphology. Our numerical experiments show that pressure is the most crucial factor in shear-under-pressure tests, with larger pressure leading to higher shearing resistance of the copolymers. The viscoelastic behaviors of hard–soft copolymers are computed from the stress autocorrelation function. The stress relaxation indicates that the soft matrix is in a rubbery state at room temperature while hard domains are “glass-like” and can be viewed as elastic solids in a macroscale model. In addition, local elastic constants of hard domains are computed using the stress–strain fluctuation method with purely local stress and local strain. Those results can be used as inputs for macroscale models for copolymers and can provide guidelines for designing polymeric materials. © 2018 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2018 , 56, 1552–1566     

Thiol‐acrylate main‐chain liquid‐crystalline elastomers with tunable thermomechanical properties and actuation strain

The purpose of this study was to investigate the influence of cross‐linking on the thermomechanical behavior of liquid‐crystalline elastomers (LCEs). Main‐chain LCE networks were synthesized via a thiol‐acrylate Michael addition reaction. The robust nature of this reaction allowed for tailoring of the behavior of the LCEs by varying the concentration and functionality of the cross‐linker. The isotropic rubbery modulus, glass transition temperature, and strain‐to‐failure showed strong dependence on cross‐linker concentration and ranged from 0.9 MPa, 3 °C, and 105% to 3.2 MPa, 25 °C, and 853%, respectively. The isotropic transition temperature (T_i) was shown to be influenced by the functionality of the cross‐linker, ranging from 70 °C to 80 °C for tri‐ and tetra‐functional cross‐linkers. The magnitude of actuation can be tailored by controlling the amount of cross‐linker and applied stress. Actuation increased with increased applied stress and decreased with greater amounts of cross‐linking. The maximum strain actuation achieved was 296% under 100 kPa of bias stress, which resulted in work capacity of 296 kJ/m³ for the lowest cross‐linked networks. Overall, the experimental results provide a fundamental insight linking thermomechanical properties and actuation to a homogenous polydomain nematic LCE networks with order parameters of 0.80 when stretched. © 2016 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2017 , 55, 157–168