The work aims to solve the problem of low polishing efficiency in traditional polishing process for aluminum alloy mobile phone shell. Grinding process for 6061 aluminum alloy was studied by using polyurethane elastic grinding wheel. Orthogonal test was performed to study the influences of abrasive particle size, feed speed, cutting depth and grinding wheel linear speed on surface roughness and material removal rate. Turning line approach was used for processing in the test, which could reduce the influence of uneven abrasive distribution. Roughness of machined surface was measured with a white light interferometer, and removal rate was obtained by calculating mass change of the workpiece in unit time. Optimal process parameters were obtained based upon comprehensive optimization of the results. In the selected 16 grinding parameters, the minimum obtainable surface roughness Ra was 44.87 nm, and the maximum removal rate was 0.329 g/min. The most important factor affecting surface roughness was abrasive particle size, and the minimum factor was feed rate. As for the material removal rate, the most important factor was cutting depth, the least was feed rate. After comprehensive optimization, the optimal combination of process parameters was: grinding wheel as 600#, speed as 2000 r/min, cutting depth as 0.04 mm, and feed rate as 20 mm/min. The application of polyurethane elastic grinding wheel to aluminum alloy grinding can improve surface quality, simplify technological process, save material preparation, installation & adjustment time, and further improve efficiency.