In this study, the material removal behaviors of diamond and SiO2 tips on lithium aluminosilicate (LAS) glass-ceramics surface were investigated in vacuum and deionized water using atomic force microscope. Two types of mechanochemical removal, stress corrosion and tribochemical removal were identified depending on counter-surface chemical activity. Their mechanisms were revealed using Fourier transform infrared spectroscopy (FTIR) and Density functional theory (DFT) calculations. In addition, combined with Raman spectra detection and thermal annealing experiments of removal areas, it was confirmed that compared with stress corrosion removal which reduced the removal energy threshold, tribochemcial removal was dominated by mechanochemical interaction without structural damage. The findings enrich the mechanochemical removal theory and furnish theoretical guidance for nano-precision machining of LAS glass-ceramic surface.