An Autonomous Self-Healing Ionic Elastomer with High Toughness Tailored for Robust Capacitive Sensors

Stretchable ionic conductors have emerged as promising materials for next-generation flexible energy and sensing devices. However, simultaneously achieving mechanical robustness, autonomous self-healing, and high ionic conductivity within one material system remains challenging. Here, we developed a tough, self-healing ionic conductive elastomer (TSHICE) based on a bioinspired, functionally partitioned design. Mimicking the hierarchical architecture of human skin, TSHICE integrates a polyether soft phase that forms continuous Li+ transport pathways with a dynamic hard phase composed of cooperative strong and weak hydrogen bonds. The dynamic hard domains act as reversible cross-linking sites, imparting mechanical integrity and efficient self-repair while maintaining reliable ionic conduction. As a result, TSHICE achieves a high fracture energy (89.8 kJ m–2), an ionic conductivity of 3.27 × 10–3 S m–1, high tensile strength (11.8 MPa), remarkable toughness (136.5 MJ m–3), rapid room-temperature self-healing, and good optical transparency. Capacitive sensors fabricated from TSHICE exhibit fast response (≈23 ms) and multisignal recognition capabilities, demonstrating strong potential for advanced sensing applications. This bioinspired design strategy offers insight into the development of ionic elastomers with integrated mechanical robustness, self-healing capability, and efficient ionic transport enabled by continuous ion-conducting pathways.