The ideal cutting-tool coating material is characterized by unique chemical and physical properties to achieve excellent cutting performance, a good thermal barrier effect, and a high-quality machined surface. Diamond-like carbon (DLC) coating, as a kind of cutting-tool coating material, has been used in cutting various materials due to its low coefficients of friction and thermal expansion, high hardness, and good chemical inert and thermal conductivity. This article mainly focuses on the modification methods for the DLC coating and their application in machining different materials. Firstly, the methods employed to improve the mechanical properties of DLC coating are reviewed and analyzed, including the multilayer structure design, transition layer, and doping other elements. Secondly, the machining performances of DLC-coated tools in the application of different materials are summarized. This review provides knowledge of modification mechanisms regarding DLC coating and its effects on mechanical properties. For machining different materials, it provides a reference to make a suitable selection and design of DLC coating to obtain better machining performance.