The escalating levels of atmospheric carbon dioxide pose a significant environmental challenge, with carbon capture and storage (CCS) from power plants being a key strategy to reduce anthropogenic CO₂ emissions. However, current capture technologies increase energy requirements by 25–40%. This review highlights the challenges and emerging materials for CO₂ capture, focusing on postcombustion, precombustion, and natural gas sweetening processes. Key advancements lie in improved materials for separations, such as solvent absorption, adsorption, and membranes, with a particular emphasis on metal–organic frameworks (MOFs). The review discusses the latest developments in these areas, emphasizing the need for molecular-level control to enhance separation efficiency and reduce costs. Despite the progress, the deployment of CCS schemes remains challenging due to the high energy penalties and economic constraints of existing capture methods. The article also reviews conventional and emerging CO₂ capture technologies, including physical absorbents, adsorption materials, and membrane-based systems, highlighting their advantages and limitations. The potential of MOFs in CO₂ capture is particularly noted, with their high surface areas, selectivity, and stability making them promising candidates for industrial applications.The escalating levels of atmospheric carbon dioxide pose a significant environmental challenge, with carbon capture and storage (CCS) from power plants being a key strategy to reduce anthropogenic CO₂ emissions. However, current capture technologies increase energy requirements by 25–40%. This review highlights the challenges and emerging materials for CO₂ capture, focusing on postcombustion, precombustion, and natural gas sweetening processes. Key advancements lie in improved materials for separations, such as solvent absorption, adsorption, and membranes, with a particular emphasis on metal–organic frameworks (MOFs). The review discusses the latest developments in these areas, emphasizing the need for molecular-level control to enhance separation efficiency and reduce costs. Despite the progress, the deployment of CCS schemes remains challenging due to the high energy penalties and economic constraints of existing capture methods. The article also reviews conventional and emerging CO₂ capture technologies, including physical absorbents, adsorption materials, and membrane-based systems, highlighting their advantages and limitations. The potential of MOFs in CO₂ capture is particularly noted, with their high surface areas, selectivity, and stability making them promising candidates for industrial applications.