We performed the (NH4)2S surface treatments before Al2O3 deposition to improve the Al2O3/III-Nitride interface quality in Al2O3/AlGaN/GaN metal-oxide-semiconductor heterostructure field-effect transistors (MOSHFETs). Interface state density at the Al2O3/GaN interface was decreased by the (NH4)2S treatment. The hysteresis width in ID-VGS and gm-VGS characteristics of the Al2O3/AlGaN MOSHFETs with the (NH4)2S treatment was smaller than that without the (NH4)2S treatment. In addition, transconductance (gm) decrease at a large gate voltage was relaxed by the (NH4)2S treatment. We also performed ultraviolet (UV) illumination during the (NH4)2S treatment for further improvement of the Al2O3/III-Nitride interface quality. Interface state density of the Al2O3/GaN MOS diodes with the UV illumination was smaller than that without the UV illumination.