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The energy storage performance of antiferroelectric ceramic capacitors has always gain much attention. Hysteresis, transition field, and polarization intensity are crucial factors influencing energy storage performance. A‐site doped small radius ions have been shown in numerous investigations to enhance the switching field, minimize hysteresis, but decrease maximum polarization intensity. How to maintain the high polarization while optimizing other parameters is a great challenge, and this problem has received scant attention in the research literature to date. In this work, Pb1‐xSrx(Zr0.54Sn0.46)0.975Nb0.02O3 (x = 0, 0.02, 0.06, 0.08, 0.1, 0.12, 0.14, 0.16, 0.20) antiferroelectric ceramics show high polarization stability. When the Sr2+ content is within 12 mol%, the saturation polarization intensity always remains at a large value (> 44μC/cm2), and the rate of change is as low as 6%. Pb0.92Sr0.08(Zr0.54Sn0.46)0.975Nb0.02O3 also displays great polarization temperature stability with a minimal change rate of 8.5% in a wide temperature range from ‐55 to 85°C. Additionally, this ceramic also has a superior energy storage performance that the recoverable energy density and energy storage efficiency and 8.95 J/cm3 and 80.4%, respectively. This work paves the way for practical simultaneous polarization and other parameter optimization. [ABSTRACT FROM AUTHOR]

(Pb,La)(Zr,Ti)O3 antiferroelectric (AFE) ceramics have attracted considerable interest due to their high‐energy storage density and numerous field‐induced phase transitions. However, the positional equilibrium of the A‐site and B‐site is typically maintained without considering that heterovalent doping of La3+ can induce defects within the material, leading to high‐temperature leakage conduction. In this work, we introduced the acceptor ion Na+ at the A‐site simultaneously and designed Pb0.9175–0.5xLa0.055NaxZr0.975Ti0.025O3 (x = 0.01, 0.03, 0.055, 0.07, 0.10) AFE ceramics. The dielectric properties of these ceramics exhibited a consistent pattern of improvement followed by deterioration as the content of Na+ increased. Notably, when x = 0.055 (Na5.5), the AFE ceramic demonstrated superior high‐temperature frequency stability with negligible leakage conduction. Impedance spectroscopy analysis suggested that Na5.5 displays the greatest resistance and highest Edc. Concurrently, the thermally stimulated depolarization current indicates that Na5.5 possesses the lowest defect concentration and the largest Ea. This can be attributed to the internal generation of defect dipole clusters (VPb′′−VO••−NaPb′−LaPb•$V_{{\mathrm{Pb}}}^{{\prime\prime}} - V_{\mathrm{O}}^{ \bullet \bullet } - {\mathrm{Na}}_{{\mathrm{Pb}}}^{\prime} - {\mathrm{La}}_{{\mathrm{Pb}}}^ \bullet $), which effectively restrict the movement of charged defects. These findings suggest that Na5.5 holds significant potential for application and offer insights into the understanding of internal defects in lead‐based AFE materials. [ABSTRACT FROM AUTHOR]