In this study we demonstrated improved electrical characteristics of Gd 2 O 3 dielectric thin films on n-GaAs substrate by manipulating wet-chemical clean and ͑NH 4 ͒ 2 S passivation. With X-ray photoelectron spectroscopy analysis, the HCl-cleaned GaAs surface was characterized to possess oxide species mainly in the form of As 2 O x near the outmost surface and Ga 2 O x with elemental arsenic close to the interface. These undesirable components could be suppressed through rinsing in NH 4 OH alkaline solution and then performing sulfidization at 80°C, resulting in alleviating the Fermi level pinning effect on Gd 2 O 3 /GaAs capacitor performance. Higher oxide capacitance and alleviated frequency dispersion at the accumulation/depletion regimes were achieved, accompanied by negligible charge trapping ͑Ͻ100 mV͒. Accordingly, gate leakage J g was lowered to ca. 10 −5 A/cm 2 at gate voltage V g = ͑V FB + 1͒ V, which was comparable to the recently reported performance of HfO 2 /GaAs structure with an ultrathin Si/Ge interfacial layer. We attributed the electrical improvements to the enhanced stabilization of high-k/sulfur-terminated GaAs interface due to abatement of native oxides and excess arsenic segregation.