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. 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 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 The dislocation density and film quality. The crystalline perfection and optical properties of GaN layers were quality by high resolution X-ray diffraction and photoluminescence.