Fabrication of Transparent,Tough, and Conductive Shape‐Memory Polyurethane Films by Incorporating a Small Amount of High‐Quality Graphene

We report a mechanically strong, electrically and thermally conductive, and optically transparent shape‐memory polyurethane composite which was fabricated by introducing a small amount (0.1 wt%) of high‐quality graphene as a filler. Geometrically large (≈4.6 μm²), but highly crystallized few‐layer graphenes, verified by Raman spectroscopy and transmission electron microscopy, were prepared by the sonication of expandable graphite in an organic solvent. Oxygen‐ containing functional groups at the edge plane of graphene were crucial for an effective stress transfer from the graphene to polyurethane. Homogeneously dispersed few‐layered graphene enabled polyurethane to have a high shape recovery force of 1.8 MPa cm⁻³. Graphene, which is intrinsically stretchable up to 10%, will enable high‐performance composites to be fabricated at relatively low cost and we thus envisage that such composites may replace carbon nanotubes for various applications in the near future.