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C−H hydroxylation of aryl acetamides and alkyl phenylacetyl esters was accomplished  via  challenging distal weak  O‐ coordination by versatile ruthenium(II/IV) catalysis. The ruthenium(II)‐catalyzed C−H oxygenation of aryl acetamides proceeded through C−H activation, ruthenium(II/IV) oxidation and reductive elimination, thus providing step‐economical access to valuable phenols. The  p ‐cymene‐ruthenium(II/IV) manifold was established by detailed experimental and DFT‐computational studies.

Insights into Ruthenium(II/IV)‐Catalyzed Distal C−H Oxygenation by Weak Coordination