. Hk; 68.55.Ac; 68.55.Jk; Structural and optical properties of high quality GaN films over the entire surfaces of sapphire substrates employing SiO 2 mask-removed double Pendeo-epitaxy technique by metalorganic chemical vapor deposition (MOCVD) were investigated by scanning electron microscopy (SEM), tranmission electron microscopy (TEM), high-resolution X-ray diffraction (HRXRD) and cathodoluminescence (CL). By optimizing the ratio of the lateral to vertical growth rate for the lateral overgrowth of the first and the second window regions of double Pendeo-epitaxial GaN layers, the crystallographic tilt in wing regions was reduced and the propagation of threading dislocations up to the surface of the GaN layers was supressed in their entire region. The luminescence properties of the GaN lyers observed by CL measurement were also improved in their entire region compared to conventional Pendeo-epitaxial growth.