As high-level equipment and advanced technologies continue toward sophistication, ultrasonic technology is extensively used in the polishing process of difficult-to-process materials to achieve efficiently smooth surfaces with nanometer roughness. The polishing of silicon carbide, an indispensable difficult-to-machine optical material, is extremely challenging due to its high hardness and good wear resistance. To overcome the current silicon carbide (SiC) ultrasonic polishing (UP) process deficiencies and strengthen the competitiveness of the UP industry, the multi-objective optimization based on the Taguchi–GRA method for the UP process with SiC ceramic to obtain the optimal process parameter combination is a vital and urgently demanded task. The orthogonal experiment, analysis of variance, grey relational analysis (GRA), and validation were performed to optimize the UP schemes. For a single objective of roughness and removal rate, the influence degree is abrasive size > preloading force > abrasive content > spindle speed > feed rate, and spindle speed > abrasive size > feed rate > preloading force > abrasive content, respectively. Moreover, the optimal process combination integrating these two objectives is an abrasive content of 14 wt%, abrasive size of 2.5 μm, preloading force of 80 N, spindle speed of 8000 rpm, and feed rate of 1 mm/s. The optimized workpiece surface morphology is better, and the roughness and removal rate are increased by 7.14% and 28.34%, respectively, compared to the best orthogonal group. The Taguchi–GRA method provides a more scientific approach for evaluating the comprehensive performance of polishing. The optimized process parameters have essential relevance for the ultrasonic polishing of SiC materials.