In this series of articles, the board members of ChemSusChem discuss recent research articles that they consider of exceptional quality and importance for sustainability. This entry features Prof. A. W. Kleij, who discusses the use of electrosynthesis to advance the regioselective hydrocarboxylation of low‐value olefins to afford high‐value carboxylic acids using carbon dioxide as reagent. In particular, in a recent breakthrough contribution a general β‐carboxylation of aromatic olefins is displayed and as such significantly expands state‐of‐the‐art carboxylation chemistry.