In the present work, cobalt-chromite-based pigment Co1-xNixCr2O4 chromate powder and nanoparticles with various transition metal concentrations (x = 0.2, 0.4, 0.6, and 0.8) were manufactured by applying aqueous synthesis approaches and sol–gel synthesis routes. XRD analysis of the powder shows that all samples formulated by the sol–gel method were crystalline with a spinel structure. Chromites show green color with a higher nickel concentration, while Co-substituent shows blackish pigments. Samples were annealed at distinct temperatures ranging from 600◦C to 750◦C. The nanoparticles obtained were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), Raman spectroscopy (RS), photoluminescence (PL), and energy-dispersive X-ray spectroscopy (EDS). The particle size of the parent compound (CoCr2O4) ranges from 100 nm to 500 nm, as measured by SEM. The tendency of particles to form aggregates with increasing annealing temperature was observed. These compounds may be successfully used as an effective doped nickel-cobalt ceramic pigment.