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The optimized [Na0.5Bi0.5−x]0.94SmxBa0.06Ti0.98W0.02O3 (i.e., NBBTW:xSm) was synthesized using conventional solid-state reactions. The structural parameters of NBBTW:xSm were revealed by PXRD and related to the Rietveld refinement. The proposed ceramic system keeps the phase structure in which the rhombohedral (R) and tetragonal (T) phases coexist due to the doping of Sm3+ and W3+ ions. The samples are likely MPB compositions, as evidenced by the SAED patterns confirming the presence of R3c and P4mm phases. The luminescence characteristics of the resulting system show a dominant absorption peak at 407 nm. This is consistent with the near UV emission of LEDs available on the market. Also, the introduction of Sm3+ ions in the NBBTW grid increases the grain size, making the ceramic system larger and more stable in the antiferroelectric region. Joncher's law of power is valid for the AC conductivity spectrum, and the activation energy (Ea) associated with relaxation and conductivity mechanism has been calculated. These results show that Sm3+ additions to NBBTW have improved their electrical and luminescence characteristics more than NBBT, making them attractive for multifunctional applications. [ABSTRACT FROM AUTHOR]