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Wide band gap II–VI nanostructures are important building blocks for new-generation electronic and optoelectronic devices. However, the difficulty of realizing p-type conductivity in these materials viaconventional doping methods has severely handicapped the fabrication of p–n homojunctions and complementary circuits, which are the fundamental components for high-performance devices. Herein, by using first-principles density functional theory calculations, we demonstrated a simple yet efficient way to achieve controlled p-type doping on II–VI nanostructures viasurface charge transfer doping (SCTD) using high work function transition metal oxides such as MoO3, WO3, CrO3, and V2O5as dopants. Our calculations revealed that these oxides were capable of drawing electrons from II–VI nanostructures, leading to accumulation of positive charges (holes injection) in the II–VI nanostructures. As a result, Fermi levels of the II–VI nanostructures were shifted toward the valence band regions after surface modifications, along with the large enhancement of work functions. In situultraviolet photoelectron spectroscopy and X-ray photoelectron spectroscopy characterizations verified the significant interfacial charge transfer between II–VI nanostructures and surface dopants. Both theoretical calculations and electrical transfer measurements on the II–VI nanostructure-based field-effect transistors clearly showed the p-type conductivity of the nanostructures after surface modifications. Strikingly, II–VI nanowires could undergo semiconductor-to-metal transition by further increasing the SCTD level. SCTD offers the possibility to create a variety of electronic and optoelectronic devices from the II–VI nanostructures viarealization of complementary doping.