A new, highly capable and dynamic aerogel adsorbent for CO2 capture was developed using a one-step sol-gel process along with solvent exchange and supercritical drying. The highest CO2 adsorption capacity in a 1% CO2 flow stream (5.55 mmol g(-1)) is much higher than other aerogel adsorbents obtained using a 10% or even higher CO2 gas mixture.