The interfacial state between the hole transport layer (HTL) and quantum dots (QDs) plays a crucial role in the optoelectronic performance of light-emitting diodes. Herein, we reported an efficient and bright green indium phosphide (InP) QD-based light-emitting diode (LED) by introducing a self-assembled monolayer of 4-bromo-2-fluorothiophenol (SAM-BFTP) molecule to improve interfacial charge transport in LED devices. The molecular dipole layer at the interface of the QD layer and HTL not only reduces the energy barrier of holes injected into QDs through vacuum energy level shift but also inhibits the fluorescence quenching of QDs caused by the HTL. Moreover, copper ions doped into phosphomolybdic acid (Cu:PMA) is selected as the hole injection layer (HIL) into the device system based on the SAM-BFTP molecule, and as a result, a green InP QD LED (QLED) with a maximum external quantum efficiency (EQE) of 8.46% and a luminance of 18 356 cd m-2 was realized. This work can inform and underpin the future development of InP-based QLEDs with concurrent high efficiency and brightness.