It is a main strategy that carbon dioxide (CO₂) in the atmosphere is effective utilized, and its concentration is balanced by capture and conversion of CO₂. Generally, CO₂ responsive polymers are prepared by alkene monomers containing amine groups. Their response and capture properties for CO₂ are improved by grafting polymerization or combining with other functional molecules. Natural polymers including polysaccharide and protein are considered as excellent candidates to prepare environmentally friendly polymers because of their rich resources, non-toxicity, biodegradability and good biocompatibility. Additional, chitosan contains a large number of amino groups, so it is employed to prepare CO₂ smart materials and exhibits specific advantages. In the current paper, firstly, CO₂ responsive polymer and chitosan(CS) are introduced. Secondly, advance in CO₂ responsive polymers and capture materials based on chitosan is reviewed. Finally, a prospect for smart materials based on chitosan in the future is provided.