The growth of sputtered GaN at low temperature is strongly desired to realize the dissemination of low-cost GaN high electron mobility transistor devices for next-generation communication technology. In this work, the roles of atomic nitrogen (N)/hydrogen (H) in GaN film growth on AlN/sapphire substrates by chemically assisted dual source sputtering are studied at a low growth temperature of 600 °C under a pressure of 2 Pa using vacuum ultraviolet absorption spectroscopy. The lateral growth was strongly enhanced with an appropriate H/N flux ratio of 1.9 at a GaN growth rate of ∼1 μm h–1. X-ray photoelectron spectroscopy measurements indicated that N removal from the grown GaN surface by atomic hydrogen promoted the migration of Ga. A smooth GaN surface was achieved at a suitable N/Ga supply ratio of 53 and a H/N ratio of 1.9 with the addition of 0.5% chlorine to the Ar sputtering gas.