Chemical mechanical polishing (CMP) was used to polish Lithium triborate (UB_3O_5 or LBO) crystal. Taguchi method was applied for optimization of the polishing parameters. Material removal rate (MRR) and surface roughness are considered as criteria for the optimization. The polishing pressure, the abrasive concentration and the table velocity are important parameters which influence MRR and surface roughness in CMP of LBO crystal. Experiment results indicate that for MRR the polishing pressure is the most significant polishing parameter followed by table velocity; while for the surface roughness, the abrasive concentration is the most important one. For high MRR in CMP of LBO crystal the optimal conditions are: pressure 620 g/cm~2, concentration 5.0 wt pct, and velocity 60 r/min, respectively. For the best surface roughness the optimal conditions are: pressure 416 g/cm~2, concentration 5.0 wt pct, and velocity 40 r/min, respectively. The contributions of individual parameters for MRR and surface roughness were obtained.