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Ceramic capacitors are receiving increasing interest because of their applications in pulsed-power devices. The perovskite oxide Bi0.5Na0.5TiO3 (BNT)-based ferroelectric ceramics are regarded as prospective lead-free candidate for dielectric capacitors because of the high polarization and outstanding relaxor behaviour. Herein, the relaxor ferroelectric (0.7−x)Bi0.5Na0.5TiO3–0.3SrTiO3–xCa0.7Sm0.2TiO3 ceramics synthesized through solid-state route and exhibited pseudocubic perovskite structure and strong relaxor behaviour. With increasing Ca0.7Sm0.2TiO3 content, the moderate permittivity and reduced grain size contributed to the monotonically increased electric breakdown strength. Among prepared samples, the x = 0.2 ceramic displayed slimmer polarization-electric field curves with a remarkable recoverable energy density (~6.8 J/cm3) and a satisfied efficiency (~82.2%) under external electric field of 450 kV/cm. Moreover, the x = 0.2 ceramic also exhibited a superb thermal reliability of energy storage properties (3.9–4.5 J/cm3 with variation of 13.3% in 25–160 °C) resulting from the diffuse phase transition. The above results make the x = 0.2 ceramics becoming promising candidates for pulsed-power devices. [ABSTRACT FROM AUTHOR]