High-entropy materials (HEMs) have managed to make their mark in the field of electrocatalysis. The flexibly adjustable component, unique configuration and proprietary core effect endow HEMs with excellent functional feature, superior stability and fast reaction kinetics. Recently, the relationship between the compositions and structures of high-entropy catalysts and their electrocatalytic performances has been extensively investigated. Based on this motivation, we comprehensively and systematically summarize HEMs, outline their intrinsic properties and electrochemical advantages, generalize current state-of-the-art synthetic methods, analyze electrochemical active centers in conjunction with characterization techniques, utilize theoretical research to conduct a high-throughput screening of the targeted high-entropy catalyst and the exploration of the reaction mechanisms, and importantly, focus specially on the electrochemical applications of high-entropy catalysts and propose strategies for regulating electronic structure to accelerate electrochemical reaction kinetics, including morphological control, defect engineering, element regulation, strain engineering and so forth. Finally, we provide our personal views on the challenges and further technical improvements of high-entropy catalysts. This work can provide valuable guidance for future research on high-entropy electrocatalysts.