MgAl2O4 was successfully used as a crystalline host network for the synthesis of nickel-based nano cyan refractory ceramic pigments. Different compositions of NixMg1−xAl2O4 (0.1 ⩽ x ⩽ 0.8) powders have been prepared by using a low temperature combustion reaction (LTCR) of the corresponding metal nitrates with urea (U) as a fuel at 300 °C in an open air furnace. The as-synthesized samples were characterized by thermal analysis (TG-DTG/DTA), X-ray powder diffraction (XRD), Fourier transform infrared spectroscopy (FTIR) and transmission electron microscopy (TEM). UV–Vis and diffuse reflectance spectroscopy (DRS) using CIE- L∗a∗b∗ parameters methods have been used for color measurements. The results show that the NixMg1−xAl2O4 samples are the crystalline phase with a particle size of 8.85–43.66 nm in the temperature range 500–1200 °C. The density, particle size, shape and color are determined for all the prepared samples with different calcination times and temperatures.