To develop novel solvent for CO2 capture, CO2 absorption performance using the aqueous of polyethylene glycol 200 (PEG200) and choline-2-pyrrolidinecarboxylic acid ([Cho][Pro]) was studied and evaluated systematically in this work, in which the critical properties of PEG200 were estimated with group contribution method, and other thermo-physical properties were determined experimentally or taken from literatures directly and then correlated with empirical equations. The CO2 solubility in PEG200 was measured and represented with the Henry’s law and Poynting correction, while the measured CO2 solubility in PEG200/H2O was correlated with RK-NRTL model. [Cho][Pro] was used as the chemical ingredient to enhance the absorption capacity and rate of CO2 in [Cho][Pro]/PEG200/H2O, and the corresponding properties and CO2 solubility were studied. The kinetic parameters, such as enhancement factor (E), reaction rate constant (k), and activation energy (Ea) of CO2 in [Cho][Pro]/PEG200/H2O were estimated from the new experimental data measured in this work and compared with the commercialized aqueous MEA solution. The process simulation and pilot-testing based on [Cho][Pro]/PEG200/H2O will be performed in the future.