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Polymer nanocomposite is a promising substitute for the charge‐storage dielectric material in capacitors. Barium titanate/polycarbonate (BT/PC) nanocomposite is one of the system due to its comprehensive excellent dielectric properties. As the dielectric response of nanocomposite depends strongly on the size of the fillers, concentration of fillers in the composite system. In this study, BT/PC nanocomposites (BT = 1‐5%) with thickness of 100 µm were fabricated to reveal the effect of the fillers on the energy storage performance of the polymer nanocomposites. Owing to the variable concentration and good dispersibility of the nanofillers, the nanocomposites with small concentration of BT particles show more uniform and denser microstructures. Moreover, with the increase of filler concentration, dielectric results indicate a breakdown strength enhancement in the nanocomposites with BT fillers, which is quite different from the nanocomposites with normal fillers, and therefore leads to the superior energy storage performance. This study demonstrates a strategy of obtaining large dielectric constants and energy densities in ceramic/polymer composites for energy storage device applications.