Due to its flexibility and versatility, robotic belt polishing is one of the most effective processing methods to improve the surface quality of aeroengine blades. Since belt polishing of blades is a material removal process aimed at reducing surface roughness, it is difficult to achieve both minimum surface roughness and maximum material removal rates. In order to solve this problem, this paper proposes an optimization method combining grey correlation analysis (GRA), the Taguchi method, and the response surface method (RSM) for the multiobjective optimization of the process parameters of Ti–6Al–4V aeroengine blade polishing. Meanwhile, the problem of the influence of asymmetry on the polishing process parameters vis-a-vis the optimization goal was solved. Experiments of robotic belt polishing for aeroengine blades were carried out. Based on the results of the principal component analysis, the grey relational grade was established to turn multiobjective optimization into single-objective optimization. A quadratic regression model of Grey correlation grade was developed, and an optimal parameter combination was obtained by the RSM. Finally, verification experiments were performed, and the combination of optimal parameters was obtained as follows: feed rate of 232.09 mm/min, compression amount of 0.08 mm, and belt line speed of 16 m/s, which reduced surface roughness by 6.29% and increased the material removal rate by 16.11%. Comparing the results of GRA-RSM and GRA, the Grey correlation grade increased by 10.96%. In other words, the goal of simultaneously reducing the surface roughness and improving the material removal rate was achieved in robotic belt polishing for aeroengine blades.