A Self‐Healing Solid‐State Ion‐Conductive Elastomer with High Mechanical Robustness and High Conductivity for Soft Ionotronics

Abstract Flexible and stretchable ion‐conductive elastomers have shown promising applications in wearable flexible sensor devices, biopotential detection, electroluminescent devices, and other areas. However, the currently employed gel‐based ion‐conductive materials encounter issues such as solvent volatilization or leakage. Herein, there is an urgent requirement to develop a solid‐state ionic conductor material that is both safe and reliable, free from issues of liquid leakage. Here, the study reports a solid‐state ion‐conductive elastomer with excellent mechanical properties and high ionic conductivity based on a synergistic strategy of multiple interaction forces. The solid‐state ion−conductive elastomer exhibits high ionic conductivity (1.42 × 10⁻⁴ S cm⁻¹ at 25 °C), superior stretchability (≈1550% elongation) and strength (1.48 MPa). Moreover, the solid‐state ion‐conductive elastomer exhibits high resilience and possesses excellent self‐healing ability. The wearable sensor, prepared based on the solid‐state ion‐conductive elastomer with excellent comprehensive performance, not only demonstrates high strain sensitivity but also captures high‐quality epidermal biopotential signals from the human body in biopotential detection. Additionally, the solid‐state ion‐conductive elastomer can serve as an electrode in ionic electroluminescent devices for human wearable applications. It is believed that the solid‐state ion‐conductive elastomer can provide novel opportunities for the advancement of wearable devices and soft ionotronics.