3D perovskites are promising to achieve efficient and bright deep‐blue light‐emitting diodes (LEDs), which are required for lighting and display applications. However, the efficiency of deep‐blue 3D perovskite‐based LEDs is limited by high density of defects in perovskites, and their deep‐blue emission is not easy to achieve due to the halide phase separation and low solubility of chloride in precursor solutions. Here, an in situ halide exchange method is developed to achieve deep‐blue 3D perovskites by spin‐coating an organic halide salts solution to treat blue 3D perovskites. It is revealed that the halide‐exchange process is mainly determined by halide ion diffusion targeting a concentration equalization, which leads to homogeneous 3D mixed‐halide perovskites. By further introducing multifunctional organic ammonium halide salts into the exchange solution to passivate defects, high‐quality deep‐blue perovskites with reduced trap density can be obtained. This approach leads to efficient deep‐blue perovskite LEDs with a peak external quantum efficiency (EQE) of 4.6% and a luminance of 1680 cd m−2, which show color coordinates of (0.131, 0.055), very close to the Rec. 2020 blue standard. Moreover, the halide exchange method is bidirectional, and blue perovskite LEDs can be achieved with color coordinates of (0.095, 0.160), exhibiting a high EQE of 11.3%.

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