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The development of advanced dielectric materials with high electric energy densities is of crucial importance in modern electronics and electric power systems. Here, a new class of multilayer‐structured polymer nanocomposites with high energy and power densities is presented. The outer layers of the trilayered structure are composed of boron nitride nanosheets dispersed in poly(vinylidene fluoride) (PVDF) matrix to provide high breakdown strength, while PVDF with barium strontium titanate nanowires forms the central layer to offer high dielectric constant of the resulting composites. The influence of the filler contents on the electrical polarization, breakdown strength, and energy density is examined. Simulations are carried out to model the electrical tree formation in the layered nanocomposites and to verify the experimental breakdown results. The trilayered polymer nanocomposite with an optimized filler content displays a discharged energy density of 20.5 J cm−3 at Weibull breakdown strength of 588 MV m−1, which is among the highest discharged energy densities reported so far. Moreover, the nanocomposite exhibits a superior power density of 0.91 MW cm−3, more than nine times that of the commercially available biaxially oriented polypropylene. The findings of this research provide a new design paradigm for high‐performance dielectric polymer nanocomposites.
Trilayered dielectric polymer nanocomposites composed of highly insulating nanosheets as the outer layers and highly polarizable nanowires as the central layer are developed to realize enhanced dielectric constant, high breakdown strength, reduced dielectric loss, and subsequently, markedly improved discharged energy densities in comparison to the conventional single‐layered thin films.