A Nd 3+ and Mg 2+ co-doped LiTaO 3 single crystal has been grown successfully by the Czochralski method. The polarized absorption spectra of the crystal were measured and investigated. The peak absorption cross-sections at 806 and 810 nm were 4.17 × 10 −20 cm 2 and 4.47 × 10 −20 cm 2 with a full width at half maximum of 29 and 17 nm for σ -and π -polarization, respectively. Based on the Judd-Ofelt theory, the spectral parameters of Nd 3+ in the as-grown crystal were investigated in detail. Moreover, the emission probabilities, branching ratio and radiative lifetime for the transitions from 4 F 3/2 were calculated. The radiative lifetime of 4 F 3/2 was calculated to be 159 µs and the luminescent quantum efficiency of the 4 F 3/2 manifold was about 81.13%. The results were also compared with other Nd 3+ doped crystals.