Increases in atmospheric carbon dioxide gas have been linked to increasing use of fossil fuels over the past century. Post-combustion capture has the greatest near-term potential for reducing CO 2 emissions. Solid sorbents provide a promising alternative to conventional amine solutions for CO 2 capture. However, practical CO 2 capture applications have been impeded primarily by limited sorbent capacity and recyclability. Here we present a novel CO 2 capture platform based on oligomeric amines supported on specially engineered mesoporous hollow particles (mesoporous capsules). This new design leads to an exceptional capture capacity of up to 7.9 mmol g -1 under simulated flue gas conditions outperforming both conventional monoethanolamine solutions and other current solid amine impregnated sorbents. In addition to their outstanding CO 2 capture capacity, the sorbents are readily regenerated at relatively low temperature and exhibit good stability and recyclability. A novel high efficiency nanocomposite sorbent for CO 2 capture has been developed based on oligomeric amines (polyethylenimine, PEI, and tetraethylenepentamine, TEPA) functionalized mesoporous silica capsules. The newly synthesized sorbents exhibit extraordinary capture capacity 10 up to 7.9 mmol g -1 under simulated flue gas conditions (pre-humidified 10% CO 2 ). The CO 2 capture kinetics were found to be fast and reached 90% of the total capacities within the first few minutes. The effects of the mesoporous capsule features such as particle size and shell thickness on CO 2 capture capacity were investigated. Larger particle size, higher interior void volume and thinner mesoporous shell thickness all improved the CO 2 capacity of the sorbents. PEI impregnated 15 sorbents showed good reversibility and stability during cyclic adsorption-regeneration tests (50 cycles).