We review the design and use of microporous polymers for pre‐ and post‐combustion capture of CO2. Microporous organic polymers are promising candidates for CO2 capture materials. They have good physicochemical stabilities and high surface areas. Ultrahigh‐surface‐area microporous organic polymers could find use in pre‐combustion capture, while networks with lower surface areas but higher heats of sorption for CO2 might be more relevant for lower pressure, post‐combustion capture. We discuss strategies for enhancing CO2 uptakes including increasing surface area, chemical functionalization to provide high‐enthalpy binding sites and the potential for pore size tuning. © 2013 Society of Chemical Industry A brief overview is given of the design and use of microporous polymers for pre‐ and post‐combustion capture processes.