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Owing to their excellent dielectric properties and energy storage performance, polymer‐based composites have shown great potential in the application of pulse energy storage capacitors and electrostatic capacitors. In this study, BaTiO3 (BT) particles with different sizes were modified with dopamine to prepare core–shell structured BT particles (PDA@BT), and then the poly(arylene ether nitrile) (PEN)‐based...