Ultra‐Tough Room‐Temperature Dielectric Switching Ionic Gels with Long‐Cycle Stability

Abstract As a favorable candidate for the next‐generation smart electronic devices, thermo‐responsive dielectric materials are faced with two crucial challenges: insufficient mechanical toughness and lack of the combination of promising dielectric switching properties, desired mechanical properties, and long‐cycle stability. Herein, a new scalable strategy is proposed for designing thermo‐responsive dielectric switching materials that simultaneously integrate the individual features, such as promising dielectric switching properties, outstanding mechanical properties, and great cycle stability, into one gel, based on a new dual dielectric switching mechanism induced by interfacial structure evolution. The ionic gel can readily achieve a superb combination of distinct reversible dielectric bistability, a high dielectric switching ratio above 150, a ≈15 °C wide thermal hysteresis loop, and tunable room‐temperature dielectric transition behavior, impressive high ductility, desirable high mechanical strength, record‐high stability of at least 1000 cycles. Such an all‐in‐one design enhances the adaptability to multiple application scenarios, durability, and a lifetime of the dielectric switching gels. Together with the facile fabrication process and recyclable thermoplastic system, thereby contributing to cost and energy saving, this research provides a feasible and sustainable strategy for constructing highly desirable thermo‐responsive dielectric switching materials.