The turn-milling methods for machining operation have been developed to increase efficiency of conventional machines recently. These methods are used especially by coupling some apparatuses on the computer numerical control (CNC) machine to decrease the production time and machine costs, ensure the maximum production and increase the quality of machining. In this study, 100Cr6 bearing steel extensively used in industry has been machined by tangential turn-milling method. This paper presents an approach for optimization of the effects of the cutting parameters including cutter speed, workpiece speed, axial feed rate, and depth of cut on the surface roughness in the machining of 100Cr6 steel with tangential turn-milling method by using genetic algorithm (GA). Tangential turning-milling method has been determined to have optimum effects of cutting parameters on the machining of 100Cr6 steel. The experimental results show that the surface roughness quality is close to that of grinding process.