Barium titanate (BaTiO3, BT) is widely used in capacitors because of its excellent dielectric properties. However, owing to its high remanent polarisation (Pr) and low dielectric breakdown field strength (Eb), achievement of high energy storage performance is challenging. Herein, a systematic strategy was proposed to reduce Pr and elevate Eb of BT via: (i) modification of the relaxor behavior by alloying it with Bi(Mg2/3Ta1/3)O3 (BMT) and (ii) heightening Eb by introducing NaTaO3 (NT) with high band gap. Consequently, the energy storage efficiency (η) of 90 % and high Eb of 780 kV cm−1 were achieved simultaneously for the BT-BMT-xNT system, which facilitated the recoverable energy density (Wrec) of 6.02 J cm−3. At 300 kV cm−1, its temperature (20–120 °C) and frequency (1–500 Hz) stabilities were found to be good. Moreover, the BT-BMT-0.15NT possessed ultrafast discharge rate (t0.9 < 51 ns) and ultrahigh power density (PD > 94 MW cm−3). This study offers an effective strategy for the design of novel high-performance dielectric energy storage materials.
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