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PVDF‐based materials have gained significant attention in the field of dielectric energy storage due to their excellent breakdown strength and energy storage density. However, the improvement has been limited by their low dielectric constant. In this article, the PVDF‐TrFE composite films with core‐shell structured (1‐x)Ba(Ti0.8Zr0.2)O3‐x(Ba0.7Ca0.3)TiO3@TiO2(BZT‐xBCT@TiO2) nanofibers were fabricated...