Mechanochemical Modification (MCM) of nanodiamond surface with DN-10 was studied in relation to the performance of nanodiamond in polishing quartz wafers. Results show that the modified nanodiamond is more stable in the pH range 8～11. A super smooth surface with an average roughness of 0.214 nm was achieved using a nanodiamond-based slurry regulated by N-(2-hydroxyethyl)ethylenediamine. It is suggested that the principal ultra-fine polishing mechanism of quartz wafer involves atom-level removal under the synergism of chemical and mechanical actions.