Dielectric capacitors attract much attention for advanced electronic systems owing to their ultra-fast discharge rate and high power density. However, the low energy storage density (Wrec) and efficiency (η) severely limit their applications. Herein, Bi0.5Na0.5TiO3-K0.5Na0.5NbO3 binary ceramic is developed to obtain excellent energy storage performance with strong relaxor behavior, together with large polarization and distorted lattice calculated by first-principles calculations. The atomic-scale local structure analysis of 0.75Bi0.5Na0.5TiO3–0.25K0.5Na0.5NbO3 ceramic reveals distorted polarization distribution and small polar nanoregion related with the enhanced relaxation and low hysteresis. Finite element analysis demonstrates ultrafine grain and increased grain boundary density following hot-pressing sintering are crucial factors in significantly enhancing the breakdown strength (Eb). As a result, ultrahigh Wrec of 12.39 J/cm3 and η of 87.1 % are achieved at a superhigh Eb of 713 kV/cm. Encouragingly, excellent performance of temperature, frequency and fatigue stability at 400 kV/cm are obtained, and high power density of ∼ 306 MW/cm3 as well as fast discharge speed of ∼ 23.3 ns are also realized. This work proposes a simple binary design with strong relaxor behavior, and highlights the potential of grain engineering to achieve outstanding energy storage performance with great stability and excellent charge-discharge property for pulse power devices.