Highly Thermally Conductive Adhesion Elastomer Enhanced by Vertically Aligned Folded Graphene

Heat and stress transfer at an interface are crucial for the contact‐based tactile sensing to measure the temperature, morphology, and modulus. However, fabricating a smart sensing material that combines high thermal conductivity, elasticity, and good adhesion is challenging. In this study, a composite is fabricated using a directional template of vertically aligned folded graphene (VAFG) and a copolymer matrix of poly‐2‐[[(butylamino)carbonyl]oxy]ethyl ester and polydimethylsiloxane, vinyl‐end‐terminated polydimethylsiloxane (poly(PBAx‐ran‐PDMS)). With optimized chemical cross‐linking and supermolecular interactions, the poly(PBA‐ran‐PDMS)/VAFG exhibits high thermal conductivity (15.49 W m(−1) K(−1)), an high elastic deformation, and an interfacial adhesion of up to 6500 N m(−1). Poly(PBA‐ran‐PDMS)/VAFG is highly sensitive to temperature and pressure and demonstrates a self‐learning capacity for manipulator applications. The smart manipulator can distinguish and selectively capture unknown materials in the dark. Thermally conductive, elastic, and adhesive poly(PBA‐ran‐PDMS)/VAFG can be developed into core materials in intelligent soft robots.