The continuous advancement in energy storage technologies necessitates the iteration of energy storage dielectrics urgently. However, the current state-of-the-art composite films fail to meet the application requirements of energy storage devices, which demand a combination of high discharged energy density (), high energy storage efficiency (), and excellent high-temperature performance. To address this challenge, we present an innovative interlayer composed of pure BN nanosheets in polyetherimide (PEI)-based asymmetrical multilayered composites doped with NaBiTiO ceramic fibers. This innovative structure confers the PEI-based composites upon synergistic optimization of polarization intensity, breakdown strength and energy loss by designed interface effectiveness adopting tailored filler and interface configuration as modulation means, which can be further confirmed by finite element simulations and comparative experiments. The resultant composite film achieves an excellent of 22.95 J cm and an ultra-high of 96.81% at ambient temperature, along with high-temperature performances of 12.88 J cm and 79.26% at 150 °C, surpassing all previously reported polymer films in terms of both metrics. This study provides new insights for developing high-performance energy storage dielectrics suitable for practical applications.
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