The control of interfacial physicochemical properties associated with device materials to minimize the impact of point defects on device performance has been a dominant theme in the semiconductor industry.The control of the density of such defects for silicon has been well established for metal oxidesemiconductor field-effect device applications through deliberate reactions with chemically congruent species, such as hydrogen. In contrast, the control of interfacial defects for technologically important III-V device materials is still an active area of research. Performance criteria for the III-V devices are demanding in terms of energy efficiency, material consumption, sensitivity, and speed. The surface reactions of III-V crystals, including the oxidation, are typically known to result in performance limitation for devices, causing significant degradation due to high defect-level densities at the surfaces/interfaces, in contrast to high quality bulk crystal regions. Here, we discuss the approach of utilizing atomically thin, ordered oxide interfacial layers of III-V compound semiconductors, since they provide a unique opportunity for metal-oxide semiconductor applications, compared to the more common approach to avoid the surface oxidation. The long-range ordered oxide interfaces have been obtained by