The present work presents the synthesis and growth conditions of (Eu,Tb):GdGa 3 (BO 3 ) 4 single crystals from a high-temperature solution Bi 2 O 3 − Ga 2 O 3 −B 2 O 3 -(Eu,Tb,Gd) 2 O 3 . Segregation coefficients of Eu 3+ and Tb 3+ doping cations were determined for the grown crystals, and their structural features, micromorphology, thermal characteristics, and luminescence properties were investigated.