Electrochemical methods offer a sustainable alternative to traditional chemical reactions, using electricity to perform molecular transformations that would otherwise require excessive heat or environmentally unfriendly reagents. However, many electrochemical reactions require an electrocatalyst to occur as they otherwise display large overpotentials at a given electrode. The use of freely diffusing redox-active molecular electrocatalysts, i.e., mediated electrocatalysis, helps lowering the overpotential for electrochemical reactions while providing precise control over the nature of the catalyst. In addition, certain molecular electrocatalysts enable transformations beyond electron transfer, for example by facilitating proton-coupled electron transfer (PCET).