Growth of GaN by MOVPE on mismatched substrates such as sapphire and SiC produces a columnar material consisting of many hexagonal grains ∼0.2–1.0 μm in diameter. However, the epitaxial–lateral-overgrowth (ELO) process for GaN creates a new material – single-crystal GaN. We have studied the ELO process using a MOVPE reactor featuring vertical gas flows and fast substrate rotation to synthesize GaN ELO samples. Characterization experiments consisted of plan-view scanning electron microscopy and vertical-cross-section transmission electron microscopy studies, which disclosed a large reduction in dislocations in the ELO regions of the GaN samples. Panchromatic and monochromatic cathodoluminescence images and spectra were employed to study the spatial variation of the optical properties of the GaN ELO samples.