A series of aminodisiloxanes were synthesized with varying degrees of functionality and steric hindrance and screened as CO2 capture solvents. Compounds with unhindered primary amine groups were found to come closest to reaching their theoretical CO2 uptake values. In contrast, materials containing either hindered primary amines or secondary amine functionality were less efficient. Addition of a cosolvent, triethylene glycol, was found in most cases to maintain solution liquidity and thereby minimize mass transfer limitations on exposure to CO2.