Lead‐free ceramic capacitors with high energy storage density are desired. Herein, the novel (1–x)(0.9Bi0.5Na0.5TiO3‐0.1SrTi0.85Zr0.15O3)‐xNa0.95Ca0.04Li0.01Nb0.96Zr0.04O3 [(1–x)(BNT‐STZ)‐xCZNNL, x = 0.1, 0.2, 0.3, 0.4 and 0.5] ceramics are prepared via citrate combustion technology and two‐step sintering method. The dense microstructures are observed and slim hysteresis loops are realized as addition of CZNNL. The enhanced recoverable energy storage density (W
re of 2.52 J cm−3) with high efficiency (η of 80%) is obtained in 0.6(BNT‐STZ)‐0.4CZNNL ceramic under a moderate electric field of 200 kV cm−1. Moreover, excellent thermal stability (W
re varies <1% and η varies <3.5%) at 20 to 100 °C) and excellent fatigue resistance are achieved for 0.6(BNT‐STZ)‐0.4CZNNL ceramic.