A method of making a single crystal GaN boule, comprising contacting a GaN seed wafer with a GaN source environment under process conditions including a thermal gradient in the GaN source environment producing growth of gallium nitride on the GaN seed wafer, thereby forming the GaN boule. The GaN source environment in various implementations includes gallium melt in an ambient atmosphere of nitrogen or ammonia, or alternatively, supercritical ammonia containing solubilized GaN. The method produces single crystal GaN boules >10 millimeters in diameter, of device quality suitable for production of GaN wafers useful in the fabrication of microelectronic, optoelectronic and microelectromechanical devices and device precursor structures therefor.