GaN metal–oxide–semiconductor structures were fabricated by atomic layer deposition of aluminum oxynitride thin films on bulk GaN substrates with c-, a-, and m-plane surfaces. Capacitance–voltage measurements ranging from 5 kHz to 1 MHz were conducted at room temperature. The interface trap number density (Nit) and interface trap level density (Dit) of the devices were extracted. A Nit of less than 2 × 1011 cm−2 and a Dit of less than 2 × 1011 cm−2 eV−1 were obtained on the a-plane and m-plane samples. Nit and Dit values were larger for c-plane samples, with the largest interface trap density observed on the c-plane sample with the highest dislocation density. The different Nit and Dit values can be attributed to different dislocation densities and dangling bond densities among different samples.