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.

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Thermo‐responsive dielectric materials are in urgent demand owing to the rapid development of smart electronic/electrical systems. Although different types and structures of thermally responsive dielectric materials have been continuously reported, their dielectric response behaviors all originate from thermodynamic phase transitions. Herein, it is demonstrated that structural relaxation in poly(vinylidene fluoride) (PVDF), a non‐thermodynamic phase transition, can induce a significant thermal dielectric pulse at room temperature. The dielectric pulse strength of up to 6.3 × 105 at 20 Hz, with a dielectric pulsing temperature of 24 °C, is achieved from polyethylene glycol (PEG)‐PVDF coaxial nanofibrous films (PVDF@PEG), fabricated via a continuous blow spinning method. Moreover, the films exhibit excellent flexibility, adjustable strength and toughness, switchable hydrophilicity/hydrophobicity, and effective thermal management capability. The relaxation‐induced dielectric pulsing effect, outstanding multifunctionality, and simple preparation combine to promote further scalability and prospects of PVDF@PEG. In particular, the work contributes to the discovery of the relaxation‐induced dielectric response mechanism, which provides a new strategy for the generation of thermo‐responsive dielectric materials.

In article number 2214544, Ming Jiang, Lijie Dong, and co-workers propose a synergistic dielectric switching mechanism. The crystallization/melting behavior of octadecane induces the aggregation/dispersion of conducting micelles, resulting in a significant simultaneous enhancement/weakening of interfacial polarization and electrode polarization-the structural transition results in an unparalleled dielectric switching effect.