Metal NPs have promising applications in catalysis. Metal active sites are usually located in the crosssections, edges, and corners of crystals and, depending on their locations, the crystals exhibit different catalytic activities. [3] Achieving maximum metal utilization by reducing the size of metal NPs to the atomic level is an effective method of improving the catalytic activity of metal catalysts. It has been found that singleatom catalysts have greatly improved catalytic performance, activity, and selectivity, and that metal single-atom catalysts (SACs) have high electrocatalytic activity and stability and are an effective strategy for achieving cost-effective catalysts for fuel cell applications. [4] An SAC was first proposed by Zhang et al. in 2011 and is defined as a carrier consisting of only isolated single atomic active sites. [1b] In recent years, SACs have emerged as having great potential for development. Their maximum atomic utilization efficiency and excellent performance have provided excellent catalytic performance in a variety of important reactions. [5] In addition, SACs have great potential in identifying and modulating the structure of the active canter to improve catalytic performance. SACs can minimize the use of noble metals and are highly advantageous in achieving 100% atomic utilization efficiency. Due to the single-atom nature of their active sites, SACs provide enhanced catalytic activity and have attracted much research attention in recent years. To avoid the agglomeration of single atoms and to achieve the separation and isolation of individual atoms, many strategies have been reported for synthesizing single atoms, such as wet chemical methods, electrochemical deposition, chemical vapor deposition, and high-temperature pyrolysis. However, it is challenging to maintain a high loading while avoiding agglomeration of individual atoms during the synthesis process. If the metal loading is too high, the high surface energy of single atoms tends to cause agglomeration of atoms. Therefore, the homogeneous dispersion and atomic size of active sites have been the focus of scientific research for decades. In general, the most common approach to preparing single-atom catalysts is to find suitable carriers to anchor single-atom metal sites (SMSs), [6] e.g., as active complexes, cations, or metal atoms) on the surface of heterogeneous carriers such as metals, metal oxides, silica, or carbon materials. However, these anchor sites are limited and disordered, leadingIn recent years, the development of alternative energy-saving, efficient, and clean catalysts for various electrochemical reactions has attracted increasing research attention. Among the various types of catalysts, singleatom catalysts (SACs) have unique properties. However, individual atoms are prone to agglomeration due to their high surface energy, which poses a major challenge to the development of SACs. Metal-organic frameworks (MOFs) have the advantages of high porosity and specific surface area, and MOF materials can be ideal ca...