A plasma enhanced atomic layer deposition (PEALD) HfO2/AlN dielectric stack was used as the gate dielectric for AlGaN/GaN metal-oxide-semiconductor high-electron-mobility transistors (MOS-HEMTs) for high-frequency power device applications. The capacitance-voltage (C-V) curves of the HfO2/AlN/GaN MOS capacitor (MOSCAP) showed a small frequency dispersion along with a very small hysteresis (>50 mV). Moreover, the interface trap density (Dit) was calculated to be 2.7 ' 1011 cm%2 V%1 s%1 at 150 °C. Using PEALD-AlN as the interfacial passivation layer (IPL), the drain current of the HfO2/AlN MOS-HEMTs increased by about 46% and the gate leakage current decreased by six orders of magnitude as compared with those of the conventional Schottky gate AlGaN/GaN HEMTs processed using the same epitaxial wafer. The 0.3-µm-gate-length HfO2/AlN/AlGaN/GaN MOS-HEMTs demonstrated a 2.88 W/mm output power, a 23 dB power gain, a 30.2% power-added efficiency at 2.4 GHz, and an improved device linearity as compared with the conventional AlGaN/GaN HEMTs. The third-order intercept point at the output (OIP3) of the MOS-HEMTs was 28 4 as compared with that of 26 5 for the conventional GaN HEMTs Overall the MOS-HEMTs with a HfO /AlN gate stack showed good potential for high-linearity RF power device applications.