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Halogenated molecules represent an important class of natural products, many of which are pharmaceutically relevant, such as chloramphenicol (antibacterial), vancomycin (antibacterial), and rebeccamycin (anticancer). Flavin-dependent halogenases have been identified as a major player in the introduction of halogen into activated organic molecules in natural product biosynthesis.[1] However, the flavin-dependent halogenases identified so far are mainly prokaryotic tryptophan halogenases with strict substrate specificity.[2–5] Most of these enzymes are involved in early biosynthetic steps of natural products to modify precursors such as tryptophan, which has limited their potential as biocatalysts to prepare various halogenated molecules. Considering the biological importance of halogens in natural products,[6] a potent halogenase able to tailor diverse complex structures will be useful for enzymatic synthesis of …