Robust Ionic Gel Elastomers Derived from Molecularly Entangled Nodes

Abstract In various types of intelligent devices, such as bionic robots, flexible polymeric elastomeric materials are essential for their operation, alongside the rigid skeleton. Conventional polymeric elastomeric materials, however, encounter a compromise between intelligence and mechanical robustness. Here, we construct ionic gel‐based elastomers that harmoniously merge high intelligence with superior mechanical attributes by employing molecularly entangled nodes that facilitate polymer chain entanglement. The entangled nodes’ dynamic interplay enables stress‐induced dissociation, promoting polymer chain slippage that effectively dissipates energy and disperses stress. Consequently, these ionic gel‐based elastomers exhibit a tensile strength of 33.5 ± 0.5 MPa and a strain capacity of 4000 ± 280%, maintaining stable performance over 7000 cycles, while also possessing the ability to detect minor material defects, thereby advancing the versatility and reliability of intelligent devices.