In this paper, we have demonstrated the optimized device performance in the Γ-shaped gate AlGaN/AlN/GaN metal oxide semiconductor high electron mobility transistor (MOS-HEMT) by incorporating aluminum into atomic layer deposited (ALD) HfO2 and comparing it with the commonly used HfO2 gate dielectric with the N2 surface plasma treatment. The inclusion of Al in the HfO2 increased the crystalline temperature (~1000 °C) of hafnium aluminate (HfAlOX) and kept the material in the amorphous stage even at very high annealing temperature (>800 °C), which subsequently improved the device performance. The gate leakage current (IG) was significantly reduced with the increasing post deposition annealing (PDA) temperature from 300 to 600 °C in HfAlOX-based MOS-HEMT, compared to the HfO2-based device. In comparison with HfO2 gate dielectric, the interface state density (Dit) can be reduced significantly using HfAlOX due to the effective passivation of the dangling bond. The greater band offset of the HfAlOX than HfO2 reduces the tunneling current through the gate dielectric at room temperature (RT), which resulted in the lower IG in Γ-gate HfAlOX MOS-HEMT. Moreover, IG was reduced more than one order of magnitude in HfAlOX MOS-HEMT by the N2 surface plasma treatment, due to reduction of N2 vacancies which were created by ICP dry etching. The N2 plasma treated Γ-shaped gate HfAlOX-based MOS-HEMT exhibited a decent performance with IDMAX of 870 mA/mm, GMMAX of 118 mS/mm, threshold voltage (VTH) of −3.55 V, higher ION/IOFF ratio of approximately 1.8 × 109, subthreshold slope (SS) of 90 mV/dec, and a high VBR of 195 V with reduced gate leakage current of 1.3 × 10−10 A/mm.