The low energy density of polymer-based dielectrics greatly limits their application in electronic components. Constructing composites with two-dimensional ceramic fillers is considered an effective strategy to increase the energy density of dielectrics because they are easily vertically distributed to the direction of the electric field. For the first time, two-dimensional KNbO 3 (KN) nanosheets with an average thickness of ∼72 nm are synthesized and applied in poly(vinylidene fluoride) (PVDF)-based dielectrics for energy storage application. Two kinds of symmetric trilayer structures including x-0-x and 0-x-0 are designed by taking advantage of interfacial polarization and the suppression of electron injection, where the number x represents the volume fraction of KN nanosheets and 0 represents pure PVDF. The results show that a 0-1-0 structured nanocomposite film with a very low loading of 1 vol % KN nanosheets achieves a high discharge energy density of 19.97 J cm −3 at 539 kV mm −1 , which is ∼109% higher than that of pure PVDF (9.56 J cm −3 at 420 kV mm −1 ). Finite element analysis (FEA) is carried out to estimate the electric field distributions in the symmetric trilayer dielectrics, confirming a consistent rule with the experimental results. This work provides guidance for designing trilayer structured dielectrics with high energy density.