The effects of composition and furnace temperature on Ni 1-Ψ Co Ψ Cr 2À2Ψ Al 2Ψ O 4 (0≤Ψ≤1) pigments prepared by Solution Combustion Synthesis were studied.As-synthesized samples showed spinel-like spongy structure, very easy to grind. However, important differences on crystallinity, crystal size, and microstructure were observed depending on composition and furnace temperature. All pigments developed intense tones, covering a wide color palette because of composition influence, although little effect was observed with furnace temperature. Stable crystalline structures, suitable grain size, and high resistance against synthesizing variables and ceramic glazes make SCS pigments perfect candidates to be used in the ceramic ink-jet decoration.