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A systematic investigation of the microstructure of CrAICχN1-χ coatings as a function of carbon contents was conducted.Quaternary CrAICχN1-χ coatings were deposited on Si wafers by a hybrid coating system combining an arc-ion plating technique and a DC reactive magnetron sputtering technique using Cr and Al targets in the Ar/N2/CH4 gaseous mixture. The effect of carbon content on microstructure of CrAICχN1-χ coatings was investigated with instrumental analyses of X-ray diffraction, X-ray photoelectron, and high-resolution transmission electron microscopy. The results show that the carbon content of CrAICχN1-χ coatings linearly increases with increasing CH4/(CH4/N2) gas flow rate ratio. The surface roughness of the CrAICχN 1-χ coating layer decreases with the increase of carbon content.