Colloidal ZnO nanoparticle (NP) films are recognized as efficient electron transport layers (ETLs) for quantum dot light-emitting diodes (QD-LEDs) with good stability and high efficiency. However, because of the inherently high work function of such films, spontaneous charge transfer occurs at the QD/ZnO interface in such a QD-LED, thus leading to reduced performance. Here, to improve the QD-LED performance, we prepared Ga-doped ZnO NPs with low work functions and tailored band structures via a room-temperature (RT) solution process without the use of bulky organic ligands. We found that the charge transfer at the interface between the CdSe/ZnS QDs and the doped ZnO NPs was significantly weakened because of the incorporated Ga dopants. Remarkably, the as-assembled QD-LEDs, with Ga-doped ZnO NPs as the ETLs, exhibited superior luminances of up to 44 000 cd/m2 and efficiencies of up to 15 cd/A, placing them among the most efficient red-light QD-LEDs ever reported. This discovery provides a new strategy for fabricating high-performance QD-LEDs by using RT-processed Ga-doped ZnO NPs as the ETLs, which could be generalized to improve the efficiency of other optoelectronic devices.