Carbon dioxide capture is regarded as an effective method of greenhouse gas reduction. Post‐combustion capture from power plants will play a key role in CO2 abatement due to their important contribution to total CO2 emissions. Compared with the state‐of‐the‐art amine scrubbing technology, adsorption‐based post‐combustion capture (PCC) possesses excellent potential for lowering energy demand, and thus the total cost. Due to their relatively weak interaction with CO2, carbons showed lower adsorption capacity during PCC as compared with some benchmark materials (e.g. amine‐based adsorbents); however, their high cyclic stability and fast adsorption/desorption kinetics suggest that carbons have the important potential to achieve an optimized or balanced performance, and thus provide a low‐cost PCC process. In this review, we present preparation options and consider the structure‐performance relationship in CO2 capture with carbons, and summarize recent progress on using carbons for CO2 capture with special focus on PCC. © 2018 Society of Chemical Industry and John Wiley & Sons, Ltd.