Aluminum optics are widely used in modern optical systems because of high specific stiffness and high reflectance. Magnetorheological finishing (MRF) provides a highly deterministic technology for high precision aluminum optics fabrication. However, the contamination layer will generate on the surface and bring difficulties for the subsequent processes, which highly limit the fabrication efficiency and precision. In this study, characteristics of the contamination layer and its formation process are firstly revealed through experimental and theoretical methods. Impurities such as abrasives are embedded into the aluminum substrate causing increasing surface hardness. The influence of the contaminant layer on machining accuracy and machining efficiency is analyzed in this study. Based on the analysis, ion beam sputtering (IBS) is induced as a contamination layer modification method. Impurities will be preferential sputtered during the process. Surface hardness and brightness will restore to the state before MRF. Moreover, the thickness of the contamination layer reduces dynamically during IBS because of the bombardment-induced Gibbsian segregation and sputter yield amplification mechanism. Consequently, we proposed a combined technique that includes MRF, IBS and smoothing polishing. Comparative experiments are performed on an elliptical shape plane surface. The results indicate that the efficiency has been increased sevenfold and surface precision is also highly improved. Our research will promote the application of aluminum optics to the visible and even ultraviolet band.