Electrocatalysis Breaking carbon-hydrogen bonds to make complex molecules has often required copious quantities of toxic oxidants. Electrochemistry offers a cleaner approach that has recently been showing great promise. Meyer et al. report a close look at how cobalt catalysis in conjunction with anodic oxidation can add methoxy groups to aryl rings. They isolated and structurally characterized a cobalt(III) complex that has cleaved the aryl carbon-hydrogen bond. Cyclic voltammetry then provided evidence for further oxidation to cobalt(IV), which accelerates formation of the carbon-oxygen bond through reductive elimination back down to cobalt(II). Angew. Chem. Int. Ed. 10.1002/anie.202002258 (2020).