Typical edge defects in the edge region of a new cemented carbide insert without edge preparation include burrs, poor surface quality, micro-breakages, and irregularities along the edge. To address the problems in new cemented carbide inserts without edge preparations, a chemical-mechanical synergistic preparation (CMSP) method for the cemented carbide insert cutting edge was proposed. Firstly, the CMSP device for the insert cutting edge was constructed. Then, the polishing slurry of the CMSP for the insert cutting edge was optimized using the Taguchi method combined with a grey relation analysis and fuzzy inference. Finally, orthogonal experiments, the Taguchi method, and analysis of variance (ANOVA) were used to investigate the effect of the polishing plate's rotational speed, swing angle, and input frequency of the controller on the edge preparation process, and the parameters were optimized. The results showed that the best parameter combination for the polishing slurry for the cemented carbide inserts was the mass concentration of the abrasive particle of 10 wt%, the mass concentration of the oxidant of 10 wt%, the mass concentration of the dispersant of 2 wt%, and the pH of 8. The CMSP process parameter combination for the linear edge had the polishing plate's rotational speed of 90 rpm, the swing angle of 6°, and the input frequency of the controller of 5000 Hz. The optimum CMSP process parameter combination for the circular edge had the polishing plate's rotational speed of 90 rpm, the swing angle of 6°, and the input frequency of the controller of 7000 Hz. The polishing plate's rotational speed had the most significant impact on the edge preparation process, followed by the swing angle, and the effect of the input frequency of the controller was the smallest. This study demonstrated that CMSP is a potential way to treat the cemented carbide insert cutting edge in a tool enterprise.