Molecular weight dependence of hybrid shish kebab structure in injection molded bar of polyethylene/inorganic whisker composites

In our previous work, a hybrid shish kebab structure, with polyethylene (PE) crystal lamellae periodically decorated on the surface of an inorganic whisker (SMCW) and aligned approximately perpendicular to the long axis of the whisker, has been observed in the injection molded bar of PE/SMCW composites. To investigate the effect of the molecular weight of the PE matrix on the formation of the hybrid shish kebab structure and the corresponding physical properties of HDPE/SMCW composites, in this work, three types of PE with different molecular weights were used to prepare the composites. They were first melt blended and then subjected to dynamic packing injection molding (DPIM), in which the prolonged shear was exerted on the melt during the solidification stage. An obvious hybrid shish kebab (HSK) structure, with PE crystal lamellae closely packed on the surface of the SMCW, was found in the samples with a low molecular weight PE (LMW-PE) matrix and a medium molecular weight PE (MMW-PE) matrix. However, in samples with a high molecular weight PE (HMW-PE) matrix, an incomplete HSK structure with PE crystal lamellae loosely decorated on the surface of the SMCW was observed. Furthermore, DSC results indicated that SMCW served as a good nucleating agent only for the composite with a LMW-PE matrix and the nucleation efficiency decreased with increasing PE molecular weight. Correspondingly, the tensile strength of the PE/SMCW composites was significantly improved by adding SMCW for the samples with a LMW-PE or MMW-PE matrix. Especially for samples with a LMW-PE matrix, the tensile strength was remarkably enhanced by the presence of only 1 wt % SMCW. For the composites with a HMW-PE matrix, the addition of SMCW had almost no reinforcing effect on the composites. The molecular weight dependence of the formation of HSK and property enhancement was discussed on the basis of the chain mobility and crystallization capability of the PE matrix.     

Insight into understanding the evolution of the epitaxy crystallization in isotactic polypropylene and polyethylene blends

In this article, epitaxial structures have been successfully obtained in the isotactic polypropylene (iPP)/polyethylene (PE) blends by an accessible injection molding methods. By studying a series of iPP/PE blends, the evolution of the epitaxial growth of PE lamellae on the oriented iPP lamellae has been detailedly discussed via wide‐angle X‐ray diffraction, small‐angle X‐ray scattering, scanning electron microscopy and differential scanning calorimetry. Unexpectedly, the exactly epitaxial angles between peculiarly arranged PE lamellae and oriented PP lamellae are all larger than the classical epitaxy theory value of 50°, and it even increases gradually with increasing PP content. It is inferred that the special crystallization of PE is the consequence of joint construction of the oriented PP crystals and the continuous intense shear field provided by pressure vibration injection molding. The epitaxial structures play a positive role in the interfacial connection between two components; thus, the mechanical properties of the blends are improved. This work provides an insight understanding on the formation mechanism of the epitaxy crystallization under shear field. Copyright © 2017 John Wiley & Sons, Ltd.     

Supercritical CO2-driven, periodic patterning on one-dimensionals carbon nanomaterials

One-dimensional carbon nano-materials, in particular carbon nanotubes (CNTs) and carbon nanofibers (CNFs), are of scientific and technological interest due to their satisfactory properties and ability to serve as templates for directed assembly. In this work, linear high density polyethylene (PE) was periodically decorated on CNTs and CNFs using a supercritical carbon dioxide (scCO₂)antisolvent-induced polymer epitaxy (SAIPE) method, leading to nano-hybrid shish-kebab (NHSK) structures. The formation mechanism of different morphologies of PE lamellae on CNTs and CNFs has been discussed. Palladium nanoparticles were synthesized and immobilized on the PE/CNF NHSK structure with the assistance of scCO₂. The obtained hierarchical nano-hybrid architecture may find applications in microfabrication and other related fields.     

Effect of cellulose nanofiber on the dynamically asymmetric phase separation in epoxy/polysulfone blends

Significant effect of cellulose nanofibers (CNFs) on cure‐induced phase separation in dynamically asymmetric system is reported. An epoxy/polysulfone blends with typical layered structure formation was chosen as the polymer matrix, and morphology evolution and rheological behavior of systems with different nano‐size fiber loadings upon curing reaction were investigated using optical microscopy and rheological measurement. CNF distributed uniformly in the polymer matrix and had good interaction with polymer chains. Curing reaction of epoxy was promoted by CNF, making the system gel and phase separate earlier. Meanwhile, system viscosity was increased with CNF addition, and the movement of polymer chains and component diffusion were constrained, as a result, the structure evolution process was slowed down. The CNF altered the final morphologies, resulting in refined structures with smaller characteristic length scales or even completely change the morphologies from the layered structures to a bicontinuous structure when the CNF concentration reached to a relatively high level. © 2019 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2019 , 57, 1357–1366     

Synthesis and characterization of polyethylene chains grafted onto the sidewalls of single‐walled carbon nanotubes via copolymerization

Polyethylene (PE) chains grafted onto the sidewalls of SWCNTs (SWCNT‐g‐PE) were successfully synthesized via ethylene copolymerization with functionalized single‐walled carbon nanotubes (f‐SWCNTs) catalyzed by rac‐(en)(THInd)₂ZrCl₂/MAO. Here f‐SWCNTs, in which α‐alkene groups were chemically linked on the sidewalls of SWCNTs, were synthesized by Prato reaction. The composition and microstructure of SWCNT‐g‐PE were characterized by means of ¹H NMR, Fourier transform infrared spectroscopy (FTIR), Raman spectroscopy, thermogravimetric analyses (TGA), field‐emission scanning electron microscope (FESEM), and transmission electron microscope (TEM). Nanosized cable‐like structure was formed in the SWCNT‐g‐PE, in which the PE formed a tubular shell and several SWCNTs bundles existed as core. The formation of the above morphology in the SWCNT‐g‐PE resulted from successfully grafting of PE chains onto the surface of SWCNTs via copolymerization. The grown PE chains grafted onto the sidewall of the f‐SWCNTs promoted the exfoliation of the mass nanotubes. Comparing with pure PE, the physical mixture of PE/f‐SWCNTs and in situ PE/SWCNTs mixture, thermal stability, and mechanical properties of SWCNT‐g‐PE were higher because of the chemical bonding between the f‐SWCNTs and PE chains. © 2007 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem 45: 5459–5469, 2007     

Correlations between microstructure of α‐row nuclei and polymorphism of shear‐induced iPP/carbon fiber cylindrite

Herein, we reported the formation mechanism of hybrid crystalline (cylindrite) in isotactic polypropylene (iPP)/carbon fiber (CF) via pulling a CF within the iPP melt. The α‐row nuclei layer closely attached to the surface of CF acts as a self‐nucleation site, rather than a heterogeneous nucleation one, to grow cylindrites. As a result, the polymorphic feature of iPP/CF cylindrite is significantly influenced by the microstructure of α‐row nuclei. With decreasing crystallization temperature (T_c), the polymorphic cylindrite changes from pure α‐form to mixed α‐/β‐form and to β‐rich form. The main characteristics of this change include: (a) the outlines of α‐row nuclei layer correspond to wave‐like, saw‐like, and straight lines; (b) the orientation level of iPP molecules in the α‐row nuclei layer become higher; (c) the α‐lamellae rearrange from loose to compact; and (d) the distance between the growth sites of β‐sectors and the surface of CF is evidently longer than in the case of α‐sectors. Moreover, this study provides a guideline for developing the interfacial enhanced iPP/CF composites through manipulation of polymorphic structure in cylindrites. © 2019 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2019 , 57, 368–377     

Synthesis and morphology of polyethylene chains grafted onto the surface of crosslinked polystyrene microspheres

The bifunctional comonomer 4‐(3‐butenyl) styrene was used to synthesize crosslinked polystyrene microspheres (c‐PS) with pendant butenyl groups on their surface via suspension copolymerization. Polyethylene chains were grafted onto the surface of c‐PS microspheres (PS‐g‐PE) via ethylene copolymerizing with the pendant butenyl group on the surface of the c‐PS microspheres under the catalysis of metallocene catalyst. The composition and morphology of the PS‐g‐PE microspheres were characterized by means of Fourier transform infrared spectroscopy, Fourier transform Raman spectroscopy, X‐ray photoelectron spectroscopy, and field‐emission scanning electron microscopy. It is possible to control the content of PE grafted onto the surface of c‐PS microspheres by varying the polymerization time or the initial quantity of pendant butenyl group on the surface of c‐PS microspheres. Investigation on the morphology and crystallization behavior of grafted PE chains showed that different surface patterns could be formed under various crystallization conditions. Moreover, the crystallization temperature of PE chains grafted on the surface of c‐PS microspheres was 6 °C higher than that of pure PE. The c‐PS microspheres decorated by PE chains had a better compatibility with PE matrix. © 2007 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem 45: 4477–4486, 2007     

Light‐driven atom transfer radical polymerization on supramolecular complexes of conjugated polymers and single‐walled carbon nanotubes

Previous approaches used to decorate latently reactive conjugated polymer‐coated carbon nanotube complexes have utilized “grafting‐to” strategies. Here, we coat the carbon nanotube surface with a conjugated polymer whose side chains contain the radical initiator, α‐bromoisobutyrate, which enables atom transfer radical polymerization (ATRP) from the polymer–nanotube surface. Using light to generate Cu(I) in situ, ATRP is used to grow narrow dispersity polymer chains from the polymer–nanotube surface. We confirm the successful polymerization of (meth)acrylates from the polymer–nanotube surface using a combination of gel permeation chromatography and infrared spectroscopy. Strikingly, we demonstrate that nanotube optoelectronic properties are preserved after radical‐mediated polymer grafting using Raman spectroscopy and photoluminescence mapping. Overall, this work elucidates a method to grow narrow dispersity polymer chains from the polymer–nanotube surface using light‐driven radical chemistry, with concurrent preservation of nanotube optoelectronic properties. © 2019 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2019, 57, 2015–2020     

The absorption and diffusion of polyethylene chains on the carbon nanotube: The molecular dynamics study

Classical molecular dynamics simulations have been used to investigate the absorption and diffusion behavior of polyethylene (PE) chains on the surface of the side‐wall of the carbon nanotube (CNT). Different degrees of polymerization from 50 to 80 at separate temperatures of 300, 400, 500, and 600 K are considered. Through the simulation, it is examined that the PE chains are absorbed on the surface of CNT and form stable composites with the nanotube as capsules. It is found that the most probable distance between the CNT and the C atoms in backbone of PE molecules only attribute to the temperature, and at T = 300 K, this distance is about 3.8 Å. Furthermore, the pattern of the composites mainly depends on the temperature and the length matching of the chains and the CNT. In particular, the PE chains keep approximately linear conformation, and extend along the axis of the CNT at the room temperature. © 2007 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys 46: 272–280, 2008     

The influence of variant PE‐b‐PEO segments on physical properties of LLDPE graft copolymers

A method was adopted to fix a series of polymers of PE‐b‐PEO with different PEO/PE segments on the chains of LLDPE. Maleic anhydride (MA) reacting with hydroxyl group of PE‐b‐PEO (mPE‐b‐PEO) was used as the intermediate. The structures of intermediates and graft copolymers were approved by ¹H NMR and FTIR. XPS analysis revealed a great amount of oxygen on the surface of grafted copolymers although the end group of PEO was fixed on the LLDPE chains through MA. Thermal properties of the graft copolymers as determined by differential scanning calorimetry (DSC) showed that PE segments in the grafted monomers could promote the heterogeneous nucleation of the polymer, increase T_c, and crystal growth rate. While the amorphous PEO segments which attached to the crystalline PE segments in LLDPE, impaired their ability to fit the crystal lattice, and depressed the crystallization of LLDPE backbones. In this study, it was also verified through the dynamic rheological data that increasing M_n of grafted monomers significantly increased the complex viscosity and enhanced the shear‐thinning behavior. Long‐branched chains formed by grafted monomers enhanced the complex moduli (G′ and G″) value and retarded relaxation rate. However, there were little influence on the rheological properties when increasing the amounts of PEO segments (or decreasing PE segments) of grafted monomers with similar molecular weight. © 2008 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys 46: 506–515, 2008     

Study on structure and performance of surface‐metallized carbon fibers reinforced rigid polyurethane composites

The simultaneous promotion in mechanical and electrical properties of rigid polyurethane (RPU) is an important task for expanding potential application. In this work, carbon fibers (CFs) reinforced RPU composites were prepared with the goal of improving mechanical and electrical properties. Metallized CFs meet our performance requirements and can be easily achieved via electrodeposition. However, the weak bonding strength in fiber‐metal‐RPU interface restricts their application. Inspired by the reducibility and wonderful adhesion of dopamine (DA), we proposed a new and efficient electrochemical method to fabricate metallized CFs, where DA polymerization was simultaneously integrated coupled with the reduction of metal ions (Ni²⁺). The characterization results helped us to gain insight about the reaction mechanism, which was never reported as far as we know. Compared with pure RPU, the tensile, interlaminar shear and impact strength of polydopamine (PDA)‐nickel (Ni) modified CFs/RPU composites were improved by 11.2%, 21.0%, and 78.0%, respectively, which attributed to the strong interfacial adhesion, including mechanical interlocking and chemical crosslinking between treated CFs and RPU. In addition, the PDA‐Ni surface treatment method also affected the dispersion of short CFs in the RPU, which increased the possibility of conductor contact and reduced insulator between fibers networks, resulting in higher electrical conductivity.     

Isothermal crystallization kinetics and melting behavior of poly(ethylene terephthalate)/barite nanocomposites

Poly(ethylene terephthalate) (PET)/Barite nanocomposites were prepared by direct melt compounding. The effects of PET‐Barite interfacial interaction on the dynamic mechanical properties and crystallization were investigated by DMA and DSC. The results showed that Barite can act as a nucleating agent and the nucleation activity can be increased when the Barite was surface‐modified (SABarite). SABarite nanoparticles induced preferential lamellae orientation because of the strong interfacial interaction between PET chains and SABarite nanoparticles, which was not the case in Barite filled PET as determined by WAXD. For PET/Barite nanocomposites, the Avrami exponent n increased with increasing crystallization temperature. Although at the same crystallization temperature, the n value will decrease with increasing SABarite content, indicating of the enhancement of the nucleation activity. Avrami analyses suggest that the nucleation mechanism is different. The activation energy determined from Arrhenius equation reduced dramatically for PET/SABarite nanocomposite, confirming the strong interfacial interaction between PET chains and SABarite nanoparticles can reduce the crystallization free energy barrier for nucleus formation. In the DSC scan after isothermal crystallization process, double melting behavior was found. And the double endotherms could be attributed to the melting of recrystallized less perfect crystallites or the secondary lamellae produced during different crystallization processes. © 2009 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys 47: 655–668, 2009     

Long‐lived layered silicates‐immobilized 2,6‐bis(imino)pyridyl iron (II) catalysts for hybrid polyethylene nanocomposites by in situ polymerization: Effect of aryl ligand and silicate modification

Heterogeneous‐layered silicate‐immobilized 2,6‐bis(imino)pyridyl iron (II) dichloride/MMAO catalysts, in which the active polymerization species are intercalated within sodium‐ and organomodified‐layered silicate galleries, were prepared for producing hybrid exfoliated polyethylene (PE) nanocomposites by means of in situ polymerization. The inorganic filler was first treated with modified‐methylaluminoxane (MMAO) to produce a supported cocatalyst: MMAO reacts with silicates replacing most of the organic surfactant, thus modifying the original crystallographic clay order. MMAO anchored to the nanoclay was able to activate polymerization iron complexes initiating the polymer growth directly from the filler lamellae interlayer. The polymerization mechanism taking place in between the montmorillonite lamellae separates the layers, thus promoting deagglomeration and effective clay dispersion. Transmission electron microscopy revealed that in situ polymerization by catalytically active iron complexes intercalated within the lower organomodified clay led to fine dispersion and high exfoliation extent. The intercalated clay catalysts displayed a longer polymerization life‐time and brought about ethylene polymerization more efficiently than analogous homogeneous systems. PEs having higher molecular masses were obtained. These benefits resulted to be dependent more on the filler nature than on the ligand environment around the iron metal center and the experimental synthetic route. © 2008 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem 47: 548–564, 2009     

Functionalization of carbon nanofibers (CNFs) through atom transfer radical polymerization for the preparation of poly(tert‐butyl acrylate)/CNF materials: Spectroscopic,thermal, morphological,and physical characterizations

Vapor‐grown carbon nanofibers (CNFs) were oxidized and functionalized for atom transfer radical polymerization (ATRP) of tert‐butyl acrylate (t‐BA) from the surface of the CNFs. The materials were characterized by solubility tests, Fourier‐transform infrared (FTIR) spectroscopy, Raman spectroscopy, thermogravimetric analysis (TGA), X‐ray diffraction (XRD), and scanning electron microscopy. The FTIR and electron microscopy results suggest that ATRP process was successfully used to graft poly(tert‐butyl acrylate) (poly(t‐BA)) chains from the surface of the fibers. Raman results strongly indicate the partial degradation of the graphitic layer of CNFs because of the chemical treatments. TGA results suggest that the presence of poly(t‐BA) leads to a decrease of the initial degradation temperature of the fibers. XRD and electron microscopy results indicate that the microstructure of fibers was not destroyed because of the oxidation and functionalization processes. © 2008 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem 46: 3326–3335, 2008     

Surface‐initiated single‐electron transfer reversible addition–fragmentation chain transfer polymerization of 2‐hydroxyethyl acrylamide on silicon substrate at ambient temperature

2‐Hydroxyethyl acrylamide was successfully polymerized via single‐electron transfer initiation on the silicon surface and propagation through the reversible addition–fragmentation chain transfer (SET‐RAFT) polymerization at ambient temperature for different polymerization times. This work is the first time application of the surface‐initiated SET‐RAFT mechanism to afford the preparation of well‐defined poly(2‐hydroxyethyl acrylamide) [poly(HEAAm)] brushes at ambient temperature. The polymerization was well controlled and produced poly(HEAAm) brushes on the silicon surface with a well‐defined target molecular weight. The controlled nature of the polymerization was further demonstrated in the presence of sulfur atoms at the chain ends in X‐ray photoelectron spectroscopy experiments. The grafting density (σ, chains nm^?2) and the average distance between grafting points (D, nm) were found to be 0.42 chains nm^?2 and 1.74 nm, respectively, indicating moderate grafting density. © 2019 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2019 , 57, 1140–1146     

Surface modification of carbon fiber for improving the interfacial adhesion between carbon fiber and polymer matrix

In this study, the reinforcing mechanism of amine functionalized on carbon fibers (CFs) has been precisely discussed, and the differences between aliphatic and aromatic compounds have been illustrated. Polyacrylonitrile‐based CFs were functionalized with ethylenediamine, 4,4‐diaminodiphenyl sulphone, and p‐aminobenzoic acid (PAB), and CF‐reinforced epoxy composites were prepared. The structural and surface characteristics of the functionalized CFs were investigated using X‐ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy (FT‐IR), and scanning electron microscopy (SEM). Mechanical properties in terms of tensile and flexural strengths and moduli were studied. The FT‐IR results confirm the success in bonding amines on the CF surface. After treatment of CFs, the oxygen and nitrogen contents as well as the N/C ratio showed an increase. XPS results provided evidence of the chemical reaction during functionalization, rather than being physically coated on the CF surface. Chemical modification of CF with diamines led to considerable enhancement in compatibility of CF filaments and epoxy resin, and remarkable improvements were seen in both tensile and flexural properties of the reinforced composites. SEM micrographs also confirmed the improvement of interface adhesion between the modified CFs and epoxy matrix. Finally, it can be concluded that PAB is a promising candidate to functionalize CF in order to improve interfacial properties of CF/epoxy composites. Copyright © 2015 John Wiley & Sons, Ltd.     

Autonomic healing of a pinhole in polyethylene and photografted polyethylene‐g‐poly(hexyl methacrylate) films

The structural changes of polyethylene (PE) and photografted polyethylene‐g‐poly(hexyl methacrylate) (PE‐g‐PHMA) with the mechanical formation of pinholes were evaluated with differential scanning calorimetry, wide‐angle X‐ray scanning, and small‐angle X‐ray scanning. The crystallinity and the long period of the lamella increased with pricking under extremely high compression stress. The partial transformation of an orthorhombic crystal into a monoclinic one was also detected. The autonomic healing of pinholes in PE and PE‐g‐PHMA was studied in detail. The degree of healing increased with an increase in the grafting ratio of poly(hexyl methacrylate) (PHMA). Three mechanisms for the healing were investigated and related to the molecular motions of PE and PHMA grafted chains, which were evaluated with dynamic mechanical analyses. © 2004 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys 42: 1705–1714, 2004     

Directional Self‐Assembly of Fluorinated Star Block Polymer Thin Films Using Mixed Solvent Vapor Annealing

We demonstrate the directional alignment of perpendicular‐lamellae domains in fluorinated three‐armed star block polymer (BP) thin films using solvent vapor annealing with shear stress. The control of orientation and alignment was accomplished without any substrate surface modification. Additionally, three‐armed star poly(methyl methacrylate‐block‐styrene) [PMMA‐PS] and poly(octafluoropentyl methacrylate‐block‐styrene) were compared to their linear analogues to examine the impact of fluorine content and star architecture on self‐assembled BP feature sizes and interdomain density profiles. X‐ray reflectometry results indicated that the star BP molecular architecture increased the effective polymer segregation strength and could possibly facilitate reduced polymer domain spacings, which are useful in next‐generation nanolithographic applications. © 2019 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2019 , 57, 1663–1672     

Morphology,thermal stability,and flammability of polymer matrix composites coated with hybrid nanopapers

In this study, a hybrid nanopaper consisting of carbon nanofiber (CNF) and polyhedral oligomeric silsequioxane (POSS) or cloisite Na⁺ clay, has been fabricated through the papermaking process. The hybrid nanopaper was then coated on the surface of glass fiber (GF) reinforced polymer matrix composites through resin transfer molding (RTM) process. The morphologies of the hybrid nanopaper and resulting nanocomposites were characterized with scanning electron microscopy (SEM). It can be seen that the nanopaper had a porous structure with highly entangled carbon nanofibers and the polyester resin completely penetrated the nanopaper throughout the thickness. The thermal decomposition behavior of the hybrid nanopapers and nanocomposites was studied with the real‐time thermogravimetric analysis/ flourier transform infrared spectrometry (TGA/FTIR). The test results indicate that the addition of pristine nanoclay increased the thermal stability of the nanopaper, whereas the POSS particles decreased the thermal stability of the nanopaper. The fire retardant performance of composite laminates coated with the hybrid nanopaper was evaluated with cone calorimeter tests using a radiated heat flux of 50 kW/m². The cone calorimeter test results indicate that the peak heat release rate (PHRR) decreased dramatically in composite laminates coated with the CNF‐clay nanopaper. However, the PHRRs of the CNF‐POSS nanopaper coated composite laminates increased. The formation of compact char materials was observed on the surface of the residues of the CNF‐clay nanopaper after cone calorimeter test. The flame retardant mechanisms of the hybrid nanopaper in the composite laminates are discussed. Copyright © 2009 John Wiley & Sons, Ltd.     

The direct architecture of carbon fiber‐carbon nanofiber hierarchical reinforcements for superior interfacial properties of CF/epoxy composites

A simple and efficient chemical method was developed to graft directly carbon nanofibers (CNFs) onto carbon fiber (CF) surface to construct a CF‐CNF hierarchical reinforcing structure. The grafted CF reinforcements via covalent ester linkage at low temperature without any usage of dendrimer or catalyst was investigated by FTIR, X‐ray photoelectron spectroscopy, Raman, scanning electron microscopy, atomic force microscopy, dynamic contact angle analysis, and single fiber tensile testing. The results indicated that the CNFs with high density could effectively increase the polarity, wettability, and roughness of the CF surface. Simultaneous enhancements of the interfacial shear strength, flexural strength, and dynamic mechanical properties as well as the tensile strength of CFs were achieved, for an increase of 75.8%, 21.9%, 21.7%, and 0.5%, respectively. We believe the facile and effective method may provide a novel and promising interface design strategy for next‐generation advanced composite structures.