An Al2O3/AlN bilayer deposited on GaN by atomic layer deposition (ALD) is employed to prepare Al2O3/AlN/GaN metal-insulator-semiconductor (MIS) diodes, and their interfacial properties are investigated using X-ray photoelectron spectroscopy (XPS) with sputter etch treatment and current-voltage (I-V) measurements. XPS analyses reveal that the native oxides on the GaN surface are reduced significantly during the early ALD stage, indicating that AlN deposition effectively clelans up the GaN surface. In addition, the suppression of Al-OH bonds is observed through the ALD process. This result may be related to the improved device performance because Al-OH bonds act as interface defects. Finally, temperature dependent I-V analyses show that the barrier height increases and the ideality factor decreases with an increase in temperature, which is associated with the barrier inhomogeneity. A Modified Richardson plot produces the Richardson constant of A** as 30.45 Acm-2K-2, which is similar to the theoretical value of 26.4 Acm-2K-2 for n-GaN. This indicates that the barrier inhomogeneity appropriately explains the forward current transport across the Au/Al2O3/AlN/GaN interface.