Extensive efforts have been devoted to improving the operational performance of quantum-dot light-emitting diodes (QLEDs). However, the fundamental understanding of the relationship between the design of the hole-injection layer (HIL)/hole-transporting layer (HTL) interface and the operational stability of QLEDs is limited. Here, we demonstrate that in the operation of red QLEDs, the leakage electrons induce in situ electrochemical reduction reactions of the polyfluorene HTLs, which in consequence create trap states and deteriorate charge-transport properties. We invoke an oxygen-plasma treatment on the PEDOT:PSS HILs, resulting in HIL/HTL interfaces with enhanced hole-injection properties. This simple method leads to more efficient exciton generation in the QDs layer and mitigated leakage electron-induced degradation of the HTLs, enabling red-emitting QLEDs with improved operational performance, i.e., high external quantum efficiency of >20.0% at a brightness ranging from 1000 to 10 000 cd m-2 and a long T95 operational lifetime of ∼4200 h at 1000 cd m-2.