The development of sapphire slurry follows the requirements of environmental friendliness, low cost and high efficiency. Therefore, the effects of KOH, aminomethyl propanol (AMP) and arginine (ARG) as pH regulators on the chemical mechanical polishing (CMP) performance of C-, A- and R-plane sapphire were investigated. The results showed that ARG was the most effective, which could increase the removal rates of C-, A- and R-plane sapphire to 5.65 µm/h, 2.80 µm/h and 3.59 µm/h, and reduce the surface roughness Sq to 0.194 nm, 0.161 nm and 0.173 nm, respectively. Mechanical action analysis, XPS, UV-Vis, and theoretical calculations revealed that ARG could improve the mechanical action of CMP and chemical action by acting as a complexing agent to complex with AlOH4−. •Combination of experiments and theoretical calculations.•A comprehensive study of pH regulators in terms of mechanical and chemical action.•Organic base ARG is a multi-purpose agent that simplifies slurry components.