We report the effects of GaN surface pretreatments on the material and electrical properties of Al2O3 dielectric deposited by atomic layer deposition (ALD). A layer of Al2O3 was deposited at different temperatures on metal organic chemical vapor deposition grown n-GaN that was treated with either H2O2:H2SO4 (1:5, piranha), HCl:H2O (1:1, HCl), or HF:H2O (1:1, HF) prior to Al2O3 deposition. The Al2O3 layers on piranha- and HF-treated GaN were observed to be uniformly smooth. The piranha pretreatment resulted in the lowest hysteresis. Pretreatment of the GaN surface with piranha removes carbon and hydroxylates the surface, resulting in better quality ALD Al2O3.