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Significance: White and co-workers report a chemoselective C(sp3)–H methylation of heterocycles by using a three-step protocol. The method was applied to a broad substrate scope, including drug molecules, peptides, and natural products. The ability to introduce a ‘magic methyl’ group in certain pharmacologically relevant compounds has been shown to significantly improve their bioactivity. Comment: The authors combined a manganesecatalyzed methylene hydroxylation with subsequent iminium/oxonium formation and methylation to achieve the functionalization of various heterocyclic cores  to the heteroatom. The transformation proceeds at low catalyst loading with remarkable chemoselectivity and moderate to good overall yields. N F3C

Manganese-Catalyzed Methylation of C(sp3)–H Bonds α to Heteroatoms