This work describes the first report of the use of an aminosilicone solvent mix for the capture of CO2. To maintain a liquid state, a hydroxyether co-solvent was employed which allowed enhanced physisorption of CO2 in the solvent mixture. Regeneration of the capture solvent system was demonstrated over 6 cycles and absorption isotherms indicate a 25–50 % increase in dynamic CO2 capacity over 30 % MEA. In addition, proof of concept for continuous CO2 absorption was verified. Additionally, modeling to predict heats of reaction of aminosilicone solvents with CO2 was in good agreement with experimental results.