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Uncontrolled massive CO2 emission into the atmosphere is becoming a huge threat to our global climate and environment. Carbon capture and storage (CCS), starting with the crucial step of CO2 capture and separation, provides a promising approach to alleviate this issue. The major challenge for CO2 capture and separation is exploring efficient adsorbent materials with high storage capacity and selectivity. This review firstly summarized the significant advancement in a variety of state-of-the-art adsorbent materials. Then, particular attention was focused on the practical strategies to enhance CO2 capture and separation based on current adsorbent materials by topological structure design, chemical doping, chemical functionalization, open metal sites, and electric fields. These strategies paved constructive ways for the design and synthesis of novel adsorbent materials. Finally, we gave a perspective view on future directions in this rapidly growing field.