Indium phosphide (InP) quantum dots have enabled light-emitting diodes (LEDs) that are heavy-metal-free, narrow in emission linewidth, and physically flexible. However, ZnO/ZnMgO, the electron-transporting layer (ETL) in high-performance red InP/ ZnSe/ZnS LEDs, suffers from high defect densities, quenches luminescence when deposited on InP, and induces performance degradation that arises due to trap migration from the ETL to the InP emitting layer. We posited that the formation of Zn 2+ traps on the outer ZnS shell, combined with sulfur and oxygen vacancy migration between ZnO/ZnMgO and InP, may account for this issue. We synthesized therefore a bifunctional ETL (CNT2T, 3′,3′″,3′″″-(1,3,5triazine-2,4,6-triyl)tris(([1,1′-biphenyl]-3-carbonitrile)) designed to passivate Zn 2+ traps locally and in situ and to prevent vacancy migration between layers: the backbone of the small molecule ETL contains a triazine electron-withdrawing unit to ensure sufficient electron mobility (6 × 10 −4 cm 2 V −1 s −1 ), and the star-shaped structure with multiple cyano groups provides effective passivation of the ZnS surface. We report as a result red InP LEDs having an EQE of 15% and a luminance of over 12,000 cd m −2 ; this represents a record among organic-ETL-based red InP LEDs.