The MnAl2O4 and CoAl2O4 nanopigments were synthesized through solution combustion method. The nanopigments extracts in the 3.5 wt% NaCl solution were prepared. Electrochemical impedance spectroscopy (EIS) and linear polarization (LP) techniques were utilized to investigate the corrosion inhibition properties of the pigments in the solutions containing pigments extracts. The epoxy nanocomposites were prepared and applied on the aluminum specimens. EIS and pull-off measurements were performed to characterize the corrosion protection properties of the epoxy nanocomposites. It was revealed that the MnAl2O4 pigment showed higher corrosion inhibition properties than CoAl2O4 in the solution phase. In addition, MnAl2O4 enhanced the corrosion resistance and decreased the adhesion loss of the epoxy coating on the aluminum substrate significantly. The MnAl2O4 nanopigment improved the corrosion resistance of the epoxy coating through increasing the barrier performance and releasing inhibitive species.