Abstract The nanoaluminate spinel Ni 1‐ x Co x Al 2 O 4 ( x = 0.0, 0.25, 0.50, 0.75, 1.0) is effectively synthesized through the use of glycine fuel utilizing a sol–gel combustion heating technique. Nanostructured nickel aluminates nonmaterials, cobalt aluminates, and their variable part spinel structures are calcinated by diligent temperature. The effect of Co 2+ ions on the NiAl 2 O 4 force network has contributed to a significant role in the modification and evolution of thermal, spectroscopic, structural, morphological, elementary, and then catalytic behaviors of cobalt‐doped nickel aluminates. It is observed that the synthesized aluminum content serves as an effective nanocatalyst for the processing of higher‐yielding organic compounds. Such methods are then checked to be effective for analyzing the premeditated processes that generated the majority of outcomes.