For the first time to the best of our knowledge, cobalt-chromium spinels CoCr_2−xGa_xO₄ with different amounts of gallium (x = 0–2 with a step of 0.5) were synthesized via the aqueous sol–gel route as ceramic pigments. The phase composition, crystallite size, morphological features, and color parameters of new compositions and their corresponding ceramic glazes were investigated using XRD, CIELab, SEM, and optical microscopy. It was demonstrated that the formation of single-phase CoCr_2−xGa_xO₄ samples was problematic. Full substitution of Cr³⁺ by Ga³⁺ ion in the spinel resulted in the formation of light blue powders, which yielded violetish blue color for the corresponding ceramic glaze.