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Metal halide perovskites have attracted extensive attention in next-generation solid-state lighting and displays due to their fascinating optoelectronic properties. However, the toxicity of lead (Pb) impedes their practical application. Herein, we report an efficient Zn-alloyed quasi-two-dimensional (quasi-2D) pure-red perovskite light-emitting device (PeLED) by introducing zinc ions (Zn2+) into the perovskite lattice and partially substituting Pb2+. The substitution of Zn2+ is confirmed by X-ray diffraction, X-ray photoelectron spectroscopy, grazing-incidence wide-angle X-ray scattering, and transmission electron microscopy measurements. In addition, the vacancy defect density of Pb and the halogen is reduced by the introduction of Zn2+ in the PEA2(Cs0.3MA0.7)2(ZnxPb1-x)3I10 perovskite system, which leads to a more ordered crystal orientation, compact morphology, and increased photoluminescence quantum efficiency. Benefiting from the improved photoelectric properties, a maximum EQE of 9.5% and a luminescence of 453 cd m-2 are achieved for the Zn-alloyed PeLEDs, with a maximum emission peak of 658 nm and stable electroluminescence spectra under various applied biases.