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Polymer dielectrics generally have comparatively low dielectric constant, operating temperatures, and/or high dielectric loss, which limits their uses especially in harsh environment. In this article, a novel trilayered nanocomposite film (TNF) was constructed via solution-casting and, subsequently, hot-pressing process, which was composed of two outer layers of polyvinylidene fluoride (PVDF, high dielectric constant) and a middle layer of polymethyl methacrylate (PMMA, high glass transition temperature, T g ). The two outer layers of TNF were filled with barium strontium titanate nanoparticles to further increase the dielectric constant of PVDF. The PMMA in the middle layer was used to largely suppress the dielectric loss and simultaneously improve the temperature tolerance of TNF. Resultsshow that the introduction of PMMA induced oriented crystal formation in the interface regions between PVDF and PMMA components. Moreover, most of the impurity ions were dramatically immobilized by partly oriented α crystals and high T g PMMA layer until the temperature exceeded 120 C. Therefore, the TNFs showed a hightemperature tolerance and notably decreased loss, which are promising for widespread energy storage applications where harsh working conditions are present.To circumvent these issues, some approaches have been proposed to promote the thermal tolerance of dielectric polymers. An effective strategy is to develop multilayer films by multilayer coextrusion, which can simultaneously achieve high-temperatureAdditional Supporting Information may be found in the online version of this article.

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Dielectric elastomers widely used for actuation applications (e.g., soft robots, tunable optics) are vulnerable to mechanical damage, so healability is crucial and related to the reliability and service lifetime of...