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In this report, we present a new approach for the fabrication and application of Cs₄PbBr₆ microcrystals (Cs₄PbBr₆ MCs). The Cs₄PbBr₆ MCs are synthesized via an anti-solvent induced crystallization of PbBr₂:CsBr directly in dimethylsulfoxide (DMSO) by introducing HBr (HBr, 48% aqueous solution). The ratio of HBr and DMSO plays a vital role in the formation of Cs₄PbBr₆. By controlling the HBr/DMSO ratio, pure Cs₄PbBr₆ or the CsPbBr₃ phase can be obtained. The Cs₄PbBr₆ MCs were initially obtained by adding HBr to CsBr:PbBr₂/DMSO. However, on increasing the amount of the added HBr, Cs₄PbBr₆ MCs were converted to CsPbBr₃ MCs and the photoluminescence (PL) disappeared. It was also found that CsPbBr₃ MCs can be transformed to Cs₄PbBr₆ MCs by simply adding DMSO to the dried CsPbBr₃ MCs. The Cs₄PbBr₆ MCs exhibit a strong PL at 516 nm with a full width at half-maximum of 25 nm …