Chemical mechanical polishing (CMP) was used to etch various GaN materials, such as GaN layers on sapphire and silicon carbide substrates grown by metal-organic chemical vapor deposition and thick GaN layers grown by physical vapor transport. It was found that CMP could reveal the dislocations in GaN surfaces due to a selective etching component. After the optimization of CMP condition, the surface finish improved and the subsurface damage was almost completely removed, demonstrated by atomic force microscopy and an electron back-scattered diffraction technique. This study established the correlation between the dislocation density and film quality. The crystalline perfection and optical properties of GaN layers were characterized by high resolution X-ray diffraction and photoluminescence.