Dielectric materials with high energy density (Ue) and breakdown strength (Eb) have played crucial roles in electronic power system and national defense weapons. However, current dielectric materials exhibit low energy storage performance, which restricts the miniaturization and lightweight of electronic devices. Herein, a novel strategy toward synchronously achieving high Ue and Eb of dielectric materials is designed by introducing low-loading poly(1,5-anthraquinone) (P15AQ) into poly(vinylidene fluoride) (PVDF). The dielectric constant (εr) match between P15AQ and PVDF promotes the uniform distribution of electric field and prevents the early breakdown damage. Meanwhile, introducing P15AQ into PVDF film improves the mechanical properties and decreases the leakage current density. As a result, Ue and Eb of the composite film reach up to 11.0 J cm− 3 and 559 MV m− 1, respectively. This work demonstrates that PVDF/P15AQ composites with remarkable comprehensive performance have the potential to achieve wider application in dielectric fields.