We demonstrate that the use of pure gallium (Ga) as a buffer layer results in improved crystal quality of GaN epilayers grown by plasma-assisted molecular beam epitaxy on c-plane sapphire. The resulting epilayers show electron Hall mobilities as high as 400 cm2/Vs at a background carrier concentration of 4 × 1017 cm−3, an outstanding value for an MBE-grown GaN layer on sapphire. Structural properties are also improved; the asymmetric (101) X-ray rocking curve width is drastically reduced with respect to that of the reference GaN epilayer grown on a low-temperature GaN buffer layer. Nitrided Ga metal layers were investigated for different Ga deposition time. These layers can be regarded as templates for the subsequent Ga main layer growth. It was found that there is an optimum Ga metal layer deposition time for improving the electron mobility in the epilayer. Heating of the Ga metal layer to the epilayer growth temperature under nitrogen plasma is found to be sufficient to produce highly oriented GaN crystals. However, nonuniform surface morphology and incomplete surface coverage were observed after nitridation of comparatively thick Ga metal layers. This is shown to be the reason for the decreasing electron mobility of the epilayers as the Ga metal layer thickness exceeds the optimum value.