Tm3+:Li3Ba2Gd3(MoO4)8 crystal has been grown by the top seeded solution growth (TSSG) method from a Li2MoO4 flux. The room temperature polarized absorption spectra, fluorescence spectra, and fluorescence decay curves of the crystal were measured. Based on the Judd-Ofelt (J-O) theory, the main spectroscopic parameters of the crystal, including the spontaneous emission probabilities, fluorescence branching ratios, and radiative lifetimes were calculated and analyzed. The broad and strong absorption bands of the crystal show that it can be efficiently pumped by the diode laser, while the large emission cross-sections of the 3F4 → 3H6 transition indicate that the crystal is a promising candidate for tunable and short pulse lasers.