Abstract Anthropogenic carbon dioxide (CO 2 ) emissions pose a significant threat to the delicate balance between human society and the natural environment. Carbon capture and sequestration is a technology designed to selectively capture CO 2 emissions generated from power plants and industrial facilities, preventing them from entering the atmosphere. Diamine‐modified metal–organic frameworks (MOFs) show promising capabilities in achieving remarkable CO 2 capacities, highlighting their potential for effective CO 2 capture applications. Herein, using MOF‐74 type frameworks, we discussed our various methodologies designed to enhance the CO 2 adsorption capacity, while also tackling the issue of maintaining structural integrity over prolonged periods, especially in humid environments. The challenges and prospects for CO 2 capture by diamine‐functionalized hydrophobic MOFs are highlighted.