ABSTRACT Phenols are abundant aromatic feedstocks widely used in organic synthesis and are commonly obtained from lignin and other renewable resources. However, the functionalization of their inert C(sp 2 )─OH bonds remains a formidable challenge, often necessitating additional preactivation steps or harsh reaction conditions. Here, we report an electrochemical strategy that enables the cleavage of phenolic C(sp 2 )─OH bonds in a formally direct manner under mild and sustainable conditions throu