We report an in situ low-damage pre-gate treatment technology in an atomic layer deposition (ALD) system prior to the ALD-Al2O3 deposition, to realize high-quality Al2O3 III nitride(III-N) interface. The technology effectively removes the poor quality native oxide on the III-N surface while forming an ultrathin monocrystal-like nitridation interlayer (NIL) between Al2O3 and III-N surface. With the pre-gate treatment technology, high-performance Al 2O3(NIL)GaN/AlGaN/GaN metal-insulator-semiconductor high-electron-mobility transistors are demonstrated, exhibiting well-behaved electrical characteristics including suppressed gate leakage current, a small subthreshold slope of ~64, and a small hysteresis of ~0.09. © 1980-2012 IEEE.