There is provided a GaN single crystal at least about 2.75 millimeters in diameter, with a dislocation density less than about 104 cm−1, and having substantially no tilt boundaries. A method of forming a GaN single crystal is also disclosed. The method includes providing a nucleation center, a GaN source material, and a GaN solvent in a chamber. The chamber is pressurized. First and second temperature distributions are generated in the chamber such that the solvent is supersaturated in the nucleation region of the chamber. The first and second temperature distributions have different temperature gradients within the chamber.