Highly Conductive Poly(Imide–Imine) Hybrid Vitrimer‐Graphene Aerogel Composites†

Comprehensive Summary Although polyimides (PIs) have shown great potential for a broad range of applications, it remains very challenging to achieve the malleability, rehealability and recyclability for PIs and their composites targeting various applications, particularly for the rapidly emerging flexible and stretchable electronics. Herein, malleable conductive poly(imide‐imine) hybrid (PIIH) vitrimer‐graphene aerogel (GA) composites have been prepared, for the first time, via simple sol‐gel film formation followed by heat‐press. The resulting PIIH‐GA composites exhibit not only the highly desired properties of thermosetting (strong mechanical strength) and thermoplastic (reprocessability) polymers, but also good conductivity enabled by the GA filler. PIIH3‐GA‐10 (with 10 wt% GA) showed one of the highest electrical conductivities (26.7 S/m) for PI‐based composites, as well as good electromagnetic interference (EMI) shielding performance. Moreover, the PIIH‐GA films could maintain good performance during stretching and even after chemical recycling, which opens new opportunities for flexible and sustainable electronics development.