The preparation technology of graphene-based coatings on cobalt-based cemented carbides and the friction properties of graphene-based coatings were researched. Based on cooling rate, growth temperature, and methane flow rate, Raman spectroscopy was used to evaluate the influence of chemical vapor deposition (CVD) on graphene-based coatings. The results show that at the growth temperature of 1000 °C, the cooling rate of 15 °C/min and methane flow rate of 10 sccm are more favorable for the growth of pure graphene coating with fewer layers on a cemented carbide surface. As methane flow boosts, the number of graphene layers increases and amorphous carbon is generated. The resulting tribological properties demonstrate that the friction coefficient of graphene-based coatings decreases as the friction load increases. The above results indicate that the graphene-based coating on a cemented carbide surface can be prepared by regulating its composition and defects through technological parameters, and it is viable to use graphene-based coating as anti-wear coating for cutting tools. The results provide a reference for the preparation and properties of cemented carbide surface graphene.