Recently, we proposed GdTaO4 as a promising high-density scintillator but the scintillation mechanism was still unknown. In this paper, we investigated the temperature-dependent luminescent properties of GdTaO4 crystal. The emission spectra are characterized by a broad band composed of two Gaussian components located at 2.2 eV and 2.7 eV of 8–300 K, which are both thermally quenched with the activation energy of 156 meV and 175 meV, respectively. These two bands are believed to be from different luminescent centers, judging from the excitation spectra, thermal activation energy and decay curves. Additionally, it was also found that the annealing atmosphere exerts little influence on the luminescence intensity. Based on the results, we tentatively assigned the high-energy band to self- trapped excitons (STE) localized in TaO3 4 groups and the low-energy band to relaxed excitons related to lattice imperfections.