Abstract: Nd3+: LiLa(MoO4)2 crystals with dimension φ20×34mm3 have been grown by Czochralski method. The spectroscopic characteristics of Nd3+:LiLa(MoO4)2 crystals were investigated. Based on Judd-Ofelt theory, the spectral parameters, such as the intensity parameters Ωλ (λ = 2, 4, 6 ), the spontaneous emission probability, the fluorescence branching ratios, the radiative lifetime and the fluorescence quantum efficiency have been obtained. The absorption cross sections are 9.52 and 4.46 ×10-20cm2 for π - and σ-polarization, respectively. The emission cross sections are 0.67 and 1.02 × 10-19cm2 for π- and σ-polarization, respectively. Under the single Xenon flash lamp pumped, the maximum pulse laser output was 74.4 mJ at 1.06μm. The laser energy threshold value Eth was 0.676J. The overall and slope efficiencies were 0.39; and 0.48;. Nd3 + :LiLa( MoO4 )2 crystal is suggested as a potential high efficient laser crystal for diode laser pumping.