To improve the laser ablation quality of polycrystalline diamond composite materials, a predictive model for each response indicator was established using the response surface methodology with laser power, scanning speed, and repetition frequency as influencing factors and ablation depth and surface roughness as response indicators. The impact patterns of the interactions of the three laser parameters on the response indicators were analyzed. Maximization of ablation depth and minimization of surface roughness were set as optimization objectives. This led to an optimized parameter combination of laser power at 94 W, scanning speed at 63 mm/s, and repetition frequency at 1490 kHz, and thereby, corresponding predicted values for the two response indicators were obtained. Subsequent secondary laser ablation experiments were conducted using the optimized parameter combination, resulting in measured errors of 1.272 μm for ablation depth and 0.134 μm for surface roughness when compared to the predicted values. The error rates between measured and predicted values were 1.59% and 17.68%, respectively, all within the specified tolerance range. This partially validates the accuracy of the model and reliability of the optimized process parameters.