Particularly, InAs NWs have been demonstrated with the impressive field-effect electron mobility (µ FE ) of higher than 10000 cm 2 V −1 s −1 when configured into single nanowire field-effect transistors (NWFETs) as well as the highly efficient visible and near-infrared photoresponse at room temperature. [2,3,9,[11][12][13]19,20] Overall, field-effect transistors (FETs) can be configured into two separate operation schemes, which are known as enhancement-mode (E-mode) and depletion-mode (D-mode). Although these two schemes are complementarily needed for the design of advanced electronic circuits, at the zero gate bias, the E-mode transistor typically operates with an OFF current, while its D-mode counterpart gives a nonzero current such that a gate voltage is needed to deplete accumulated carriers to achieve the OFF state of devices. Therefore, the E-mode transistor is primarily preferred for the energy-efficient and large-scale circuit integration. [14][15][16][17] However, most of the III-V NWs consist of significant amounts of surface/interface traps, originating from the native oxide and/or unoptimal interface associating with high-κ dielectrics directly deposited on the top, which yield the accumulation layer on NWs' surface pining the Fermi level above the conduction band or below the valence band. [14,[16][17][18] Even though the different diameter, Recently, III-V semiconductor nanowires (NWs) are widely investigated as field-effect transistors (FETs) for high-performance electronics, optoelectronic, and others; nevertheless, effective control in their device performances, especially the threshold voltage is still not well attained, which can potentially limit their practical uses for technological applications. This study reports a simple but highly reliable metal-oxide nanoparticle (NP) surface decoration approach onto the device channel in order to manipulate electrical characteristics of III-V NWFETs, such as the threshold voltage and transistor operation, through the manipulation of free electrons in the NW channel (i.e., InAs, InP, and In 0.7 Ga 0.3 As) via depositing various metal-oxide NPs with different work functions. Without any passivation layer, this decoration approach can yield the stable NW device characteristics in ambient. Notably, the versatility of our decoration scheme has also been illustrated through the realization of highperformance enhancement-mode InAs NW-paralleled-arrayed devices as well as the configuration of highly efficient InAs NW NMOS inverters, comprising of both depletion and enhancement mode devices. All these results further elucidate the technological potential of this decoration approach for future high-performance, low-power nanoelectronic device fabrication, and circuit integration.