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In recent years, single‐atom catalysts (SACs) have received increasing attention in the field of electrochemical CO2RR with their efficient atom utilization efficiency and excellent catalytic performance. However, their low metal loading and the presence of linear relationships for single active sites with simple structures possibly restrict their activity and practical applications. Active site tailoring at the atomic level is a visionary approach to break the existing limitations of SACs. This paper first briefly introduces the synthesis strategies of SACs and DACs. Then, combining previous experimental and theoretical studies, this paper introduces four optimization strategies, namely spin‐state tuning engineering, axial functionalization engineering, ligand engineering, and substrate tuning engineering, for improving the catalytic performance of SACs in the electrochemical CO2RR process by combining previous experimental and theoretical studies. Then it is introduced that DACs exhibit significant advantages over SACs in increasing metal atom loading, promoting the adsorption and activation of CO2 molecules, modulating intermediate adsorption, and promoting C−C coupling. At the end of this paper, we briefly and succinctly summarize the main challenges and application prospects of SACs and DACs in the field of electrochemical CO2RR at present. [ABSTRACT FROM AUTHOR]

Excess CO2 can be effectively converted into valuable fuels and chemicals by electrochemical CO2 reduction, which can help establish a low‐carbon emission economy and solve the current energy crisis. In recent years, metal‐organic frameworks (MOFs), as an emerging multifunctional material with porous structure, high chemical tunability and large specific surface area, has received increasing attention in the field of electrochemical CO2RR. In this paper, we present a comprehensive overview of various MOFs and their derivatives as CO2RR electrocatalysts and analyze their roles in the catalytic process from physical and chemical aspects. In addition, combining experiments and theory, this article also offers a personal view on the electronic structure modulation strategies to improve electrocatalytic performance. The article concludes with an analysis of the challenges in realizing MOFs and their derivatives for electrocatalytic CO2RR applications. [ABSTRACT FROM AUTHOR]