The intrinsic toxicity-free indium phosphide (InP) quantum dots (QDs) are regarded as the most promising alternative to the heavy metal-containing QDs for quantum dot light-emitting diodes (QLEDs) in next-generation display and lighting applications. Here, a stepwise hole injection layer consisting of PEDOT:PSS and solution-processed molybdenum oxide is employed to improve the hole injection for solution-processed green QLEDs based on InP/ZnSe/ZnS colloidal QDs. The hole transport layer (HTL) of poly(vinylcarbazole) with high-lying LUMO level is further used to block electrons. As a result, the electron-hole recombination zone is restricted in the middle of the InP/ZnSe/ZnS QDs emissive layer, reducing the possibility of exciton quenching at HTL and/or the HTL/QDs interface. This enables high-efficiency green InP-based QLEDs with the peak external quantum efficiency, current efficiency, and luminance of 5.84%, 20.8 cd/A, 5145 cd/m <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sup> , respectively.