The orthogonal polarized dual-wavelength laser has attracted increasing attention due to its unique applications in spectral analysis, differential radar, terahertz, etc. In this paper, the Nd-doped LiY(MoO 4 ) 2 (LYMO) crystal with a disordered structure is selected as a laser gain medium to obtain the dual-wavelength laser. The fluorescence spectra of the Nd:LYMO crystal show obvious polarization anisotropy, which is caused by the anisotropic lattice field. The πand σ-polarized stimulated emission cross-sections at 1061 and 1068 nm are calculated to be 17.5