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Highly efficient lead halide perovskites with tunable emission performance have become new candidate materials for light‐emitting devices and displays; however, the toxicity of lead and instability of halide perovskites greatly limits their application. Herein, rapid and large‐scale synthesis of highly emissive organic–inorganic manganese halide perovskites, (C5H6N)2MnBr4 and C5H6NMnCl3, are presented by a one‐pot solution‐based method, of which (C5H6N)2MnBr4 displays a high absolute photoluminescence quantum yield (95%) in the solid‐state. The developed (C5H6N)2MnBr4 perovskite noticeably exhibits high stability. Therefore both as‐synthesized green and red emissive manganese‐based phosphors with superior optical properties are used to fabricate blue light pumped white light‐emitting diodes (WLEDs), displaying excellent quality white light with a high color rendering index value of 91 and a correlated color temperature of 5331 K. This study not only presents the robust large‐scale production synthetic approach for organic–inorganic manganese halide perovskites, but also facilitates the development of high‐performance phosphors for future lighting and display technologies.

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