A series of high-capacity, amine impregnated sorbents based on a cost-effective silica foam with ultralarge mesopores is reported. The sorbents exhibit fast CO 2 capture kinetics, high adsorption capacity (of up to 5.8 mmol g À1 under 1 atm of dry CO 2 ), as well as good stability over multiple adsorptiondesorption cycles. A simple theoretical analysis is provided relating the support structure to sorbent performance.