ABSTRACT Ultra‐stretchable conductive elastomers with low‐hysteresis recovery and anti‐creep capability are indispensable for high‐fidelity wearable sensors and human‐machine interaction systems. Conventional carbon nanotube (CNTs)‐based elastomers rely on weak physical interactions between CNTs and polymer matrices, failing to achieve robust chemical bonding and thus suffering from severe interfacial slippage. Here, we report a novel dechlorination‐triggered nano‐welding strategy to construct a 3D C─C covalent bonding network between CNTs and silicone polymers. Through thermodynamically favorable dechlorination of polyvinyl chloride (PVC)‐derived chlorinated graphene‐decorated CNTs (Cl‐G/CNTs), a nano‐welded interface is in‐situ formed via synchronous covalent linkage and nanoscale mechanical interlocking. The resulting conductive elastomer exhibits exceptional stretchability of more than 870%, low‐hysteresis recovery of 99.9%@25% strain, remarkable anti‐creep performance of 10000 cycles). This high‐performance elastomer has been successfully fabricated into high‐resolution sensors, including wearable physiological monitors and an underwater piezometer with reliable depth‐resolving capability (∼100 Pa). Our innovation breaks the intrinsic trade‐off between organic–inorganic interfacial integration and mechanical‐electrical synergy, establishes an ultra‐stretchable and low‐hysteresis conductive elastomer for high‐fidelity wearable sensing.
Ren et al. (Wed,) studied this question.