High-quality and high-efficiency processing of gallium nitride (GaN) crystals is urgently required for optoelectronic communications and other major industries. This study proposes a novel high-efficiency non-damage magnetorheological chemical polishing (MCP) process to overcome the existing problems of low efficiency and lattice distortion during processing. The effects of the MCP fluid composition and key processing parameters on the surface roughness and material removal rate (MRR) of GaN crystals were studied experimentally. The results showed that a compounded abrasive containing silica fluid exhibited better polishing effects than a single abrasive. The polishing efficiency could be improved by adding NaOH solid particles, and the MRR reached 13.19 nm min−1 when the pH of the MCP fluid was 10. The MRR increased gradually with an increase in the pole rotation speed and worktable speed and a decrease in the polishing gap. The surface roughness of the GaN crystals was improved from Ra 115 nm to Ra 0.375 nm after polishing for 4 h. The surface and sub-surface damage of the polished GaN crystals was analyzed using scanning electron microscope and transmission electron microscope. The results confirmed that the MCP process can realize the non-damage polishing of GaN crystals. Moreover, a prediction model for the surface roughness of GaN crystals in the MCP process was constructed. The overall difference between the actual and predicted surface roughness values for the model was 11.6%.
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