Clay‐bonded SiC supported cobalt oxide catalysts were produced by the aerosol‐assisted metal organic chemical vapor deposition method (AA‐MOCVD) using Co(acac)₂ as precursor. Deposition temperatures 270 and 300 °C were the most appropriate for the synthesis of a composite catalyst of high activity for the CO conversion reaction. A cone‐shaped crystal habit is the dominant morphology. The catalysts were decorated with Au nanoparticles (NPs) of sizes in the range of 5-10 nm. This substantially improved the activity of the catalysts, lowering the onset temperature of activity by about 50 °C. Ambient‐pressure X‐ray photoelectron spectroscopy (APXPS) was used to investigate in situ the electronic state of cobalt and gold during CO oxidation. APXPS results show that while Au remains in the metallic state during the reaction, it enhances the reduction of Co³⁺ to Co²⁺. Au NPs adsorb CO molecules from the gas phase and supply them to the neighbor cobalt oxide particles.