In this study, two pollution-free approaches were used to improve the processing efficiency of mechanical chemical polishing (MCP) for sapphire substrates. The first was dedicated to polishing using synthetic silica abrasives with high reactivity as soft abrasives, and the second was dedicated to polishing using organic acids and bases as catalysts on the polishing pad and coolant, including citric acid, theophylline, green tea, and coffee. The results showed that the rate of material removal of MCP with highly reactive silica abrasives was more than 187.5% larger than that of pristine silica abrasives with low reactivity, and surface roughness was 21% smaller than that of pristine silica abrasives. Meanwhile, in case of citric acid, the removal mass of sapphire was more that 29.2% larger than that of an original polishing method, and surface roughness was about 15.2% smaller than that of original polishing method. However, theophylline, green tea, and coffee affected processing efficiency negligibly or negatively, due to a limited effect on increasing the pH level of the coolant, and the powder residue in the coolant obstructing the contact between the nano-silica abrasive particles and sapphire surface. These results indicate that highly reactive nano-silica abrasives and citric acid show good catalytic activity towards the sapphire processing efficiency of MCP. The promoting mechanism of highly active silica abrasives and citric acid for the processing efficiency of MCP is also discussed in detail in this study.