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Recently, quasi-two-dimensional (Q-2D) perovskites have received much attention due to their excellent photophysical properties. Phase compositions in Q-2D perovskites have obvious effect on the device performance. Here, efficient green perovskite light-emitting diodes (PeLEDs) were fabricated by employing o-fluorophenylethylammonium bromide (o-F-PEABr) and 2-aminoethanol hydrobromide (EOABr) as the mix-interlayer ligands. Phase compositions are rationally optimized through composition and interlayer engineering. Meanwhile, non-radiative recombination is greatly suppressed by the introduction of mix-interlayer ligands. Thus, green PeLEDs with a peak photoluminescence quantum yield (PLQY) of 81.4%, a narrow full width at half maximum (FWHM) of 19 nm, a maximum current efficiency (CE) of 27.7 cd/A, and a maximum external quantum efficiency (EQE) of 10.4% were realized. The results are expected to offer a feasible method to realize high-efficiency PeLEDs.