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Barium Strontium Titanate (Ba 1-x Sr x TiO 3 , BST) possesses the advantages of high permittivity, low remnant polarization and dielectric loss, suggesting great potential in the application of power capacitors. However, the low maximum polarization severely restricts the achievement of outstanding energy storage properties (ESP). Herein, we design a lead-free bulk ceramic: (1-x)Ba 0. 55 Sr 0 · 45 TiO 3 -xBi 0.5 Na 0. 5 TiO 3 [(1-x)BST-xBNT] (x = 0.1–0.4), prepared by two-step solid-state reaction method. The introduction of BNT contributes to (1) the boost of maximum polarization (from 21 μC/cm2 up to 32.6 μC/cm2) due to Bi3+ lone pair covalent effect (2) strong relaxor behavior (1.71≪ γ 1.84) derived from weakly coupled nanopolar regions, which can be verified by high activation energy E a = 0.341 eV at x = 0.3, improves the ESP and thermal stability of the ceramics. According to the above strategies, high W rec = 1.73 J/cm3 and η = 84.4% are achieved in the 0.7BST-0.3BNT ceramics at 206 kV/cm, which is preferable to the previous results regarding BST-based bulk ceramics. The excellent thermal stability (20–120 °C), frequency stability (1–500 Hz), as well as anti-fatigue characteristic (cycling number: 105) were obtained in the 0.7BST-0.3BNT. Furthermore, 0.7BST-0.3BNT ceramics exhibit high-power density (P D = 44.9 MW/cm3) and rapid discharge rate (t 0.9 = 99.2 ns) from 20 °C to 120 °C. This work provides a feasible way to achieve good energy storage and charge-discharge properties for pulse power energy storage systems. [ABSTRACT FROM AUTHOR]