Nd3+:Bi2(MoO4)3 single crystal grown by the Czochralski technique was oriented and the orientation relationship between the principal axes of the optical indicatrix (X, Y, Z) and the crystallographic axes (a, b, c) was determined. The polarized absorption spectra, polarized fluorescence spectra, and fluorescence decay curve of the crystal were measured at room temperature. The Judd-Ofelt theory and the Fuchtbauer-Landenburg formula were applied to analyze the spectroscopic parameters. The relation between the spectral properties and the crystal structure was discussed. A primary laser output of about 235 mW at 1064 nm with the slope efficiency of 25% has been obtained under a Ti:sapphire laser pumping.