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Flexible nanocomposite dielectrics with high dielectric constant and discharge energy density have broad application prospects in the field of energy storage. However, dielectrics with high dielectric constant tend to have a high dielectric loss. Herein, we prepared a dielectric composite material with ultra‐high discharge energy density by modifying the interface between nanoparticles and poly(vinylidene fluoride‐co‐hexafluoropropylene) (P[VDF‐HFP]). After coating a shell of insulating amorphous SiO2 (~7 nm) outside the barium titanate (BT), the electric field concentration and current density inside BT particles can be significantly reduced. In addition, coating the SiO2 shell with a polydopamine (PDA) shell (~7 nm) not only enhances the interface interaction between the nanoparticles and the polymer matrix, but also can form lots of microcapacitors in the composite. As a result, an ultra‐high discharge energy density of 13.78 J/cm3 at the expense of relatively inconspicuous efficiency (~59.8%) in the BT@SiO2@PDA/P (VDF‐HFP) with 2.5 wt% loading has been achieved under 460 kV/mm. This is mainly attributed to the increases of dielectric constant from 12.1 to 14.2 and the relatively low dielectric loss (0.086) at 100 Hz. Moreover, compared with the pure P (VDF‐HFP) (400 kV/mm), the breakdown voltage of the composite with 2.5 wt% loading is surged to 460 kV/mm, which benefited from the hindrance of nanoparticles on carrier migration at low content. This work has realized a thin‐film dielectric with ultra‐high discharge energy density through a novel design of the nanoparticle structure, providing a theoretical direction for the development of polymer dielectric capacitors. [ABSTRACT FROM AUTHOR]