CO2 removal from mixed CO2-N-2 gas was investigated by using aqueous solutions of monoethanolamine (MEA) (10 wt %), glycerol (10 wt %), and a mixture of MEA (10 wt %)-glycerol (10 wt %) in a pilot-scale packed column. An Aspen Plus simulator was employed to simulate the CO2-MEA-glycerol process using a rate-based model. Then, the experimental data of the pilot-scale columns were applied to validate the simulation results. The lowest and highest rich CO2 loadings for the MEA solvent were measured in 3.65 and 13.9% mol CO2/mol MEA with 1.4 and 3.9 L/min gas flow rates, respectively. In comparison to the CO2-MEA system, the lowest and highest rich CO2 loadings for the CO2-MEA-glycerol system increased by 42.2 and 14.8%, respectively, under the same conditions. The values of CO2 loadings predicted by the simulation were in concordance with the experimental values. The results showed that the hybrid MEA-glycerol solution had a better CO2 absorption performance than the aqueous MEA solution.