The material yttrium aluminum oxide (Y3Al5O12) is one of the materials commonly used in laser devices. For application in optical devices, it is necessary to produce ultra-precise surface quality, however, Y3Al5O12 material belongs to the group of difficult-to-machine materials with high brittleness and hardness. Therefore, it is very difficult to ensure that the main criterion when finishing this material to produce a quality surface in the nanometer form with the ability to remove the material is very difficult. To solve this problem, this work provided a new chemical - mechanical polishing mixture. The proposed polishing mixture of ZrO2, Na2SiO3–5H2O, and MgO abrasives has a weight ratio of 8%, 5% and 1% respectively, with the remainder being deionized water. The surface result after polishing is obtained with a material removed rate of 38 (nm/min) along with an ultra-smooth surface produced with Ra = 0.41 nm. With the help of X-ray photoelectron spectroscopy (XPS) method before and after polishing by CMS, the reaction mechanisms were elucidated. Analytical results show that Y3Al5O12 material produces YOOH and AlOOH in Na2SiO3 solution, then combines with –Si–OH to form (Y-Si) and (Al-Si) with significantly reduced hardness compared to other Y3Al5O12 materials, these products combine with MgO to form montmorillonites (3MgO–Al2O3–3SiO2–3Y2O3–5Al2O3). With this formation, the surface layer of Y3Al5O12 material becomes soft and is easily removed by ZrO2 abrasive particles under the influence of mechanical polishing, resulting in superfine surfaces are generated from the proposed CMS model.