The polycrystalline Nd3+-doped rare earth orthotantalate LuTaO4 was synthesized with high temperature solid-state reaction method, and the structure was determined by applying the Rietveld refinement to its x-ray diffraction. Also, the emission and excitation spectra at 7.6 K have been analyzed. The free-ions and crystal-field parameters were fitted to the experimental energy levels with the root mean square deviation of 14.6 cm−1. According to the crystal-field calculations, 152 Stark energy levels of Nd3+ were assigned. Finally, the fitting results of free-ions and crystal-field parameters were compared with those already reported for Nd3+:YAlO3. The results indicate that the free-ions parameters are similar to those of the Nd3+ in LuTaO4 and YAlO3 hosts except for the values of two-body electrostatic parameter γ, and the 2-rank crystal-field parameters of two hosts have relatively large differences while other crystal-field parameters have been similar to each other. Moreover, the crystal-field interaction of Nd3+ in LuTaO4 is stronger than that in YAlO3.