TlGa1−xSbxS2 (x = 0.0, 0.2, 0.4, 0.6, 0.8, 1.0) single crystals were grown using the Bridgman–Stockbarger method. The direct energy gaps of the single crystals were found to be 2.586, 2.459, 2.344, 2.228, 2.119, and 1.987 eV for the composition x = 0.0, 0.2, 0.4, 0.6, 0.8, and 1.0, respectively, at 20 K. The indirect energy gaps were found to be 2.479, 2.357, 2.232, 2.118, 1.983, and 1.871 eV for the composition x = 0.0, 0.2, 0.4, 0.6, 0.8, and 1.0, respectively, at 20 K. The optical energy gaps decreased linearly with increasing composition x. The temperature dependence of the optical energy gaps for each of the single crystals was well fitted with the Varshni equation.