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The supporting electrolyte is an essential component of electrochemical reactions. Although there have been many reports on the influence of the type of electrolyte and its concentration on reaction efficiency in electrosynthesis, very few reports have systematically discussed the reasons for such effect. In several reaction systems, we have found that the coordination of anions from the supporting electrolyte to cationic organic species generated in electrochemical oxidation dramatically changes the reaction efficiency. In this comprehensive paper, we review these case studies, generalize the findings learned from them, and provide guidelines for strategic electrolyte design.