Nd 3+ :Li 3 Ba 2 Gd 3 (MoO 4 ) 8 crystal has been grown from a Li 2 MoO 4 flux by the top seed solution growth method (TSSG). The structure of the crystal was confirmed by X-ray powder diffraction. The principal coefficients of thermal expansion along a, b and c-axes were precisely measured to be 1.62×10 −5 , 1.73×10 −5 and 2.15×10 −5 K −1 , respectively. The specific heat value was 0.42J/gK at 50°C. The polarized spectral properties of Nd 3+ :Li 3 Ba 2 Gd 3 (MoO 4 ) 8 crystal were investigated and the spectroscopic parameters were calculated and analyzed based on the Judd–Ofelt theory. The absorption cross-sections around 805nm were determined to be 15.13, 3.84 and 5.27×10 −20 cm 2 for E//b, E//D1 and E//D2, respectively. The emission cross-sections σ em were determined to be 9.5×10 −20 cm 2 for E//b, 8.2×10 −20 cm 2 for E//D1, and 7.9×10 −20 cm 2 for E//D2, respectively. The fluorescence lifetime was measured to be 130μs and the quantum efficiency was calculated to be 93%.