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Due to the demands of miniaturization, weight reduction and green development for electronic devices, development of lead-free dielectric ceramic capacitors with high recoverable energy density (W rec) and energy storage efficiency (η) attracts much attention. To this end, (1- x)[0.75(Na 0.5 Bi 0.5)TiO 3 -0.25SrTiO 3 ]- x NdNbO 4 (abbreviated as: NBST- x NN) ceramics were fabricated through a solid-state reaction method. After adding NN, the non-perovskite phase of Bi 2 Ti 2 O 7 (BTO) with low dielectric constant (ε r) and loss (tan δ) is generated. Finite element software (COMSOL) was used to explore the influence of the BTO phase on breakdown strength (E b). The simulation result indicates that the BTO phase with a low ε r concentrates a larger local electric field (LEF), and thus weakens the LEF loading in the main perovskite phase, which is beneficial for enhancing E b. Moreover, NN doping significantly decreases the oxygen vacancy concentration in NBST ceramics, which plays a key role in improving E b. On the other hand, as NN content increases, the hysteresis of the polarization (P)-electric field (E) loops is substantially suppressed, and the polarization saturation is delayed, which can be ascribed to the appearance of the BTO phase having a linear dielectric characteristic and to the enhanced fluctuations of composition and charge by NN doping. Benefitting from the above factors, the optimal energy storage performance (ESP) with a W rec of 4.14 J/cm3 and an η of 90 % is obtained in NBST-0.08NN ceramics. Meanwhile, the ESP of NBST-0.08NN ceramics shows good charge-discharge properties and thermal stability. In conclusion, these results demonstrate that NBST-0.08NN ceramics are promising candidates as environment-friendly dielectric capacitor materials. [ABSTRACT FROM AUTHOR]