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By designing an orthogonal experiment with four factors and three levels, (Na0.5Bi0.495Nd0.005)TiO3 (NBT‐Nd) nanopowders were prepared using a hydrothermal method under different conditions to determine the optimum hydrothermal synthesis conditions. The synthesized NBT‐Nd nanopowders were characterized using X‐ray diffraction measurement, ultraviolet–visible spectra, photoluminescence spectra, and transmission electron microscopy to evaluate the orthogonal experimental conditions. The results showed that NBT‐Nd powders with excellent crystalline and luminescence properties could be obtained at 160°C, with a 16 h reaction time, 8 mol·L−1 NaOH, and with 0.4489 g C19H42BrN. The optimized hydrothermal method‐prepared NBT‐Nd powder has a rather pure rhombohedral perovskite structure at room temperature, and exhibits an aggregated polycrystalline structure containing nanotubes and nano‐sized particles. Under excitation of 247 nm light, strong fluorescence emissions are excited at 423 nm and 441 nm in the NBT‐Nd powder that were generated by transitions of Nd3+ from 2D5/2 to 4I9/2 and from 4G11/2 to 4I9/2, respectively. Through CIE1931 chromaticity calculation of the emission peaks, the NBT‐Nd powder was shown to emit indigo blue fluorescent light. [ABSTRACT FROM AUTHOR]