To fine-tune surface ligands towards high-performance devices,wedeveloped an in situ passivation process for all-inorganic cesium lead iodide (CsPbI 3)perovskite quantum dots (QDs) by using ab ifunctional ligand, L-phenylalanine (L-PHE). Through the addition of this ligand into the precursor solution during synthesis,the in situ treated CsPbI 3 QDs displays ignificantly reduced surface states,i ncreased vacancy formation energy,h igher photoluminescence quantum yields, and muchi mproved stability.C onsequently,t he L-PHE passivated CsPbI 3 QDs enabled the realization of QD solar cells with an optimal efficiency of 14.62 %a nd red light-emitting diodes (LEDs) with ah ighest external quantum efficiency (EQE) of 10.21 %, respectively,d emonstrating the great potential of ligand bonding management in improvingt he optoelectronic properties of solution-processed perovskite QDs.