AbstractThe persistent increase in atmospheric carbon dioxide (CO2) concentration poses a significant contemporary challenge. Contemporary chemistry is heavily focused on sustainable solutions, particularly the photo‐/electrocatalytic reduction of CO2 and its utilization for energy storage. Despite promising prospects, efficient chemical CO2 conversion faces obstacles such as ineffective CO2 uptake/activation and catalyst mass transport. Covalent organic frameworks (COFs) have emerged as potential catalysts due to their precise structural design, functionalizable chemical environments, and robust architectures. COF‐based materials, especially those incorporating diverse active sites like single metal sites, metal nanoparticles, and metal oxides, hold promise for CO2 conversion and energy storage. This review sheds light on CO2 photoreduction/electroreduction and storage in Li‐CO2 batteries catalyzed by COF‐based composites, focusing on recent advancements in integrating COFs with nanoparticles for CO2 reduction. It discusses design principles, synthesis methods, and catalytic mechanisms driving the enhanced performance of COF‐based nanocomposites across various applications, including electrochemical reduction, photocatalysis, and lithium CO2 batteries. The review also addresses challenges and prospects of COF‐based catalysts for efficient CO2 utilization, aiming to steer the development of innovative COF‐based nanocomposites, thus advancing sustainable energy technologies and environmental stewardship. © 2024 Society of Chemical Industry and John Wiley & Sons, Ltd.