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Sn‐based materials are identified as promising catalysts for the CO₂electroreduction (CO2RR) to formate (HCOO⁻). However, their insufficient selectivity and activity remain grand challenges. A new type of SnO₂nanosheet with simultaneous N dopants and oxygen vacancies (V_O‐rich N‐SnO₂NS) for promoting CO₂conversion to HCOO⁻is reported. Due to the likely synergistic effect of N dopant andV_O, theV_O‐rich N‐SnO₂NS exhibits high catalytic selectivity featured by an HCOO⁻Faradaic efficiency (FE) of 83% at−0.9 V and an FE of>90% for all C1 products (HCOO⁻and CO) at a wide potential range from −0.9 to−1.2 V. Low coordination Sn–N moieties are the active sites with optimal electronic and geometric structures regulated byV_Oand N dopants. Theoretical calculations elucidate that the reaction free energy of HCOO* protonation is decreased on theV_O‐rich N‐SnO₂NS, thus enhancing HCOO⁻selectivity. The weakened H* adsorption energy also inhibits the hydrogen evolution reaction, a dominant side reaction during the CO2RR. Furthermore, using the catalyst as the cathode, a spontaneous Galvanic Zn‐CO₂cell and a solar‐powered electrolysis process successfully demonstrated the efficient HCOO⁻generation through CO₂conversion and storage.

Single atom catalysts (SACs) are considered as the emerging catalysts for boosting electricity‐driven CO₂reduction reaction (CRR) and hydrogen evolution reaction (HER). To replace the rare and expensive noble metal electrocatalysts, developing nonprecious metal SACs (NPMSACs) with superior electrocatalytic activity and stability is of paramount importance for achieving high efficiency in CRR and HER. Herein, a brief overview of recent achievements in the carbon‐rich NPMSACs for both CRR and HER is provided. The synthesis strategies and corresponding electrocatalytic performances of various carbon‐rich NPMSACs are discussed in the order of various metals (Ni, Co, Fe, Zn, and Sn for CRR, as well as Ni, Co, Fe, Mo, and W for HER), with a special attention paid to understand the structure–activity relationships. Finally, the remaining challenges and future perspectives for enhancing CRR and HER performance of NPMSACs are outlined.