New NixMg1−xAl2O4 nanosized in different composition (0.1 ≤ x ≤ 0.8) powders have been synthesized successively for first time by using low temperature combustion reaction (LTCR) of corresponding metal chlorides, carbonates and nitrates as salts with 3-methylpyrozole-5-one (3MP5O) as fuel at 300 °C in open air furnace. Magnesium aluminate spinel (MgAl2O4) was used as crystalline host network for the synthesis of nickel-based nano ceramic pigments. The structure of prepared samples was characterized by using different techniques such as thermal analysis (TG–DTG/DTA), X-ray powder diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR) and transmission electron microscopy (TEM). UV/Visible and Diffuse reflectance spectroscopy (DRS) using CIE-L*a*b* parameters methods have been used for color measurements. The obtained results reveal that NixMg1−xAl2O4 powder of samples is formed in the single crystalline and pure phase with average particle size of 6.35–33.11 nm in the temperature range 500–1200 °C. The density, particle size, shape and color are determined for all prepared samples with different calcination time and temperature.