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GdScO 3 single crystal codoped with Tm3+ and Tb3+ ions was successfully grown by the Edge-defined Film-fed Growth Method (EFG) for the first time. Absorption, fluorescence spectrum and fluorescence lifetimes of the grown crystal at room temperature were measured. The absorption cross-section at 789 nm was calculated to be 8.20 × 10−21 cm2. The emission cross-section was 1.35 × 10−21 cm2 at 1504 nm with the FWHM of 95.3 nm. The fluorescence lifetimes of the 3H 4 state and the 3F 4 state were fitted to be 253 μs and 1460 μs, respectively. Compared with Tm3+ single doped GdScO 3 crystal, the codoping of Tb3+ successfully depopulated the 3F 4 energy level and enhanced the emission at 1.5 μm region. It indicated that Tm,Tb:GdScO 3 could be favorable laser medium for 1.5 μm-laser operation. • Tm3+ and Tb3+ co-doped GdScO 3 crystal was successfully grown by the edge-defined film-fed method (EFG) for the first time. • Spectral parameters and Judd-Ofelt parameters of Tm,Tb:GdScO3 crystal were obtained and compared. • The fluorescence mechanism of Tm3+ and Tb3+ co-doped GdScO 3 crystal has been studied. [ABSTRACT FROM AUTHOR]