We prepared Nd-doped CaYAl3O7 single crystals with different Nd concentrations of 0.1, 0.5, 1.0, 5.0, 10, and 20% by the floating zone method. Photoluminescence (PL) and scintillation properties of all the samples were investigated, and the performance as near-infrared (NIR) scintillators was evaluated. All the samples exhibited some luminescence peaks of 4f-4f transitions of Nd3+ in PL and scintillation spectra at around 890, 1060, and 1300 nm. The 5.0% Nd-doped sample showed the highest PL quantum yield of 49.5%. In addition, the 5.0% Nd-doped sample had the highest scintillation intensity under X-ray irradiation among the samples, and the lowest detectable dose rate was 0.001 Gy/h.