The possibility of chemical mechanical polishing (CMP) as an intermediate ex-situ surface planarization process for thin-film epitaxy devices has been investigated. The surface quality of the homoepitaxial GaN after a surface pretreatment of CMP on the GaN-on-sapphire template drastically improved as compared to that with the regular homoepitaxial process. In addition, it was found that CMP contributed to a reduction in the dislocation densities in the subsequent homoepitaxial GaN layers. The CMP-treated GaN surface exhibited pits, with an average diameter of 0.3 μm, due to the chemical etching effect of the CMP slurry. These pits are thought to enhance the epitaxial lateral over growth of the GaN thin films, leading to a reduction in the dislocation densities in the homoepitaxial GaN layers.