0.05, 0.1, 0.5, and 1% Nd-doped CsI single crystals were synthesized by the vertical Bridgman-Stockbarger method, and the photoluminescence and scintillation properties were evaluated. Under X-ray irradiation, two emission peaks were observed at 310 and 430 nm ascribed to on- and off-center configuration self-trapped excitons, respectively. In near-infrared regions, sharp peaks were observed at 900, 1080, and 1350 nm due to 4F3/2-4I9/2, 4F3/2-4I11/2, and 4F3/2-4I13/2 transitions of Nd3+, respectively. Dose rate response functions had good linearity in the range of 0.06–6 Gy/h in all the samples, and the 0.5% Nd-doped sample showed the highest intensity among all the samples.