Dielectric capacitors play a crucial role in the field of energy storage; however, the low discharged energy density () of existing commercial dielectrics limits their future applications. Currently, further improvement in the of dielectrics is constrained by the challenge of simultaneously achieving high permittivity (ε) and high breakdown electric field strength (). To address this issue, we designed a series of four-layer poly(vinylidene fluoride) (PVDF)-based composite films comprising three functional layers: a sodium bismuth titanate (NBT) plus PVDF composite (NBT&PVDF) layer to achieve high ε values and a pure PVDF layer and a boron nitride (BN) plus PVDF composite (BN&PVDF) layer to achieve high values. This design synergistically enhanced the ε and values of the composite films by exploiting low-loss macrointerface polarization via adjustment of the functional layer stacking order, as supported by simulation analyses. Ultimately, the composite film with a topmost layer of pure PVDF, followed by an NBT&PVDF layer, another pure PVDF layer, and a BN&PVDF layer achieved an enhanced value of 26.42 J·cm and excellent efficiency of 80.03% at an ultrahigh value of 770 MV·m. This approach offers an innovative pathway for developing advanced energy storage composite dielectrics via macrointerface manipulation.
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