The upsurge in the exploitation of state-of-the-art spin-induced electrocatalysts has been witnessed recently for sustainable energy and related conversion engineering. In this regard, several modification strategies based on the spin structure–activity relationship have been proposed for the rational design of spin electrocatalysts. The electron transfer and orbital interactions between the catalysts and reactants/intermediates exhibit spin independence, stimulating the regulation of the spin configuration of electrocatalysts for renewable conversion-related electrocatalytic reactions. This review discusses the recent advances in spin-related catalysts to provide an insightful view of the origins of the enhanced catalytic activity. After clarifying the fundamental principle between spin-related mechanisms and electrocatalytic properties, we summarize recent attempts to regulate spin states to optimize electrocatalytic performance by classifying several regulation strategies, including theoretical and experimental means. In addition, we demonstrate the important role of regulating the spin configuration in electrocatalytic applications by giving several representative examples of catalysts. Finally, a summary and outlook on the existing problems and the future development of spin-related electrocatalysis are further presented.