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In this paper, Sm-doped 0.96(K0.48Na0.52)(Nb0.95Sb0.05)–0.04Bi0.5(Na0.82K0.18)0.5ZrO3 (abbreviated as KNSN–0.04BNKZ) lead-free piezoelectric ceramics were prepared by conventional solid-state sintering method and the effects of Sm2O3 on the phase structure, microstructure, electrical and luminescent properties of KNSN–0.04BNKZ potteries were studied. Results revealed that a single solid solution phase with pseudo-cubic perovskite structure was formed between KNSN–0.04BNKZ and Sm2O3. Existence of weak dielectric/ferroelectric properties with a diffuse dielectric anomaly and slim P–E hysteresis loops of the Sm-doped KNSN–0.04BNKZ demonstrated the ferroelectric relaxor behavior of the KNNS–0.04BNKZ–xSm ceramics. Accordingly, the temperature stability and fatigue behavior of the modified ceramics were significantly improved. It was found that the KNSN–0.04BNKZ ceramics with 0.002 mol Sm addition exhibited nearly temperature independent properties and fatigue-free behavior. Moreover, Sm-modified KNSN–0.04BNKZ exhibits a bright photoluminescence with a strong orange emission under visible light irradiation. As a material with both electrical and luminescent properties, it has good application prospect in future optoelectronic components by integrating its luminescent and electrical properties.