A 2,3,4,6-tetrafluoro-7,7,8,8,-tetracyanoquinodimethane (F4-TCNQ) doping interlayer was developed to improve charge imbalance and the efficiency in indium phosphide (InP)-based quantum dot light-emitting diodes (QLEDs). The doping layer was coated between a hole injecting layer (HIL) and a hole transport layer (HTL) and successfully diffused with thermal annealing. This doping reduces the hole injection barrier and improves the charge balance of InP-based QLEDs, resulting in enhancement of an external quantum efficiency (EQE) of 3.78% (up from 1.6%) and a power efficiency of 6.41 lm/W (up from 2.77 lm/W). This work shows that F4-TCNQ interlayer doping into both HIL and HTL facilitates hole injection and can provide an efficient solution of improving charge balance in QLED for the device efficiency.