A comparison was made of 6H-SiC surfaces etched with H2, C2H4/H2, and HCl/H2, and the resulting crystal quality of epitaxial GaN films deposited on these substrates. To remove the many fine scratches and to smooth the rough surfaces typical of commercial SiC substrates, the Si-face 6H-SiC substrates were etched in H2, C2H4/H2, and HCl/H2 at 145 °C. GaN was subsequently deposited on these etched surfaces after first depositing a low temperature GaN buffer layer via metalorganic chemical vapor deposition (MOCVD). The surface morphologies after etching and after GaN deposition were characterized by atomic force microscopy and Normaski differential interference contrast microscopy, while the crystal quality of the GaN films was assessed by double crystal x-ray rocking curves and x-ray topography. 6H-SiC substrate surfaces were improved in terms of the removal of scratches and the reduction of surface roughness, and both surface morphology and crystal quality of the subsequently deposited GaN films were enhanced. However, the dislocation density was not decreased by the surface etching. The best GaN film was produced by etching the substrate in pure H2 for 40 minutes before growth. Recommendations for the optimum substrate treatment are made.