Chromium-carbon films were deposited by utilizing reactive high-power impulse magnetron sputtering with different mixture ratios of ethyne and argon with a constant deposition total pressure while the deposition temperature, pulse frequency, duty cycle and average power of the chromium cathode remain the same. The microstructure and chemical bonding of the obtained films within different composition were compared. The results show that with the increasing ethyne ratio, the carbon content in films increases linearly with two slopes. Moreover, the microstructure of the deposited film changes from a dense glassy structure into a columnar structure, even a clusters structure. The sp2-C bonding in films decreases but the Cr–C bonding increases with decreasing the ethyne ratio. This reveals the main phase of films changes from a hydrogenated amorphous carbon phase into a glassy amorphous chromium carbide phase. Such changes of the microstructure and phase cause a large difference on the film hardness and elasticity.