Dielectric polymer materials with high energy density and low dielectric loss are highly desired for applications in advanced electronic devices and electric power systems. Here, we report on flexible dielectric composites using semiconductor nanoparticles as fillers and polyvinylidene fluoride (PVDF) as a matrix. The introduction of a small amount of ZnO filler results in significantly enhanced voltage breakdown strength and energy density in comparison with pure PVDF. Based on the multi-core model, combining the electric double layer theory and the interface contact theory, we investigate mechanisms and come out with that transportation of carriers under applied voltage is regulated by the charged interface, which delays the formation of the conduction path. Besides, the electric field imposed on the composites is alleviated by the internal micro-electric field.