Single-atom site catalysts (SACs) have made great achievements due to their nearly 100% atomic utiliza-tion and uniform active sites.Regulating the surrounding environment of active sites,including electron structure and coordination environment via atom-level interface regulation,to design and construct an advanced SACs is of great significance for boosting electrocatalytic reactions.In this review,we system-ically summarized the fundamental understandings and intrinsic mechanisms of SACs for electrocatalytic applications based on the interface site regulations.We elaborated the several different regulation strate-gies of SACs to demonstrate their ascendancy in electrocatalytic applications.Firstly,the interfacial elec-tronic interaction was presented to reveal the electron transfer behavior of active sites.Secondly,the different coordination structures of metal active center coordinated with two or three non-metal ele-ments were also summarized.In addition,other atom-level interfaces of SACs,including metal atom-atom interface,metal atom-X-atom interface (X:non-metal element),metal atom-particle interface,were highlighted and the corresponding promoting effect towards electrocatalysis was disclosed.Finally,we outlooked the limitations,perspectives and challenges of SACs based on atomic interface regulation.