AbstractElectroluminescence of colloidal nanocrystals promises a new generation of high-performance and solution-processable light-emitting diodes. The operation of nanocrystal-based light-emitting diodes relies on the radiative recombination of electrically generated excitons. However, a fundamental question—how excitons are electrically generated in individual nanocrystals—remains unanswered. Here, we reveal a nanoscopic mechanism of sequential electron-hole injection for exciton generation in nanocrystal-based electroluminescent devices. To decipher the corresponding elementary processes, we develop electrically-pumped single-nanocrystal spectroscopy. While hole injection into neutral quantum dots is generally considered to be inefficient, we find that the intermediate negatively charged state of quantum dots triggers confinement-enhanced Coulomb interactions, which simultaneously accelerate hole injection and hinder excessive electron injection. In-situ/operando spectroscopy on state-of-the-art quantum-dot light-emitting diodes demonstrates that exciton generation at the ensemble level is consistent with the charge-confinement-enhanced sequential electron-hole injection mechanism probed at the single-nanocrystal level. Our findings provide a universal mechanism for enhancing charge balance in nanocrystal-based electroluminescent devices.