The development of dielectric capacitors toward high voltage and high power density requires materials with excellent insulation and energy storage performances. In this work, a polymer dielectric with polyetherimide (PEI) as the matrix and calcium barium zirconate titanate (BZCT) coated by barium titanate fiber (BT) as the filler (BZCT@BT) was constructed. The (0.5%-10% BZCT@BT/PEI) polymer dielectric has an excellent discharge energy density (Ue) of 6.66 J/cm3 and maintains an advanced charge/discharge efficiency (η) of 93.29% when the BT content was 0.5% and the BZCT particle content was 10%. The addition of BZCT endows the polymer dielectric with a higher relative dielectric constant (εr), while BT, maintaining a lower εr than BZCT, could reduce the electric field (E) distortion caused by the dielectric mismatch between PEI and BZCT. Oriented fiber fillers increase the breakdown strength of the polymer dielectric, ultimately increasing the performance of energy storage. A new strategy for the design of energy storage polymer dielectrics was provided by this work.
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