Solvent-based post-combustion carbon capture (PCC) is a mature and essential technology to solve the global warming problem. The high energy consuming issue and the flexible operation required by the power plants inquire about the development of effective control systems for PCC plants. This study proposes the optimal-based control approach that utilizes optimal set-point values for the quality controllers. The five optimal-based control schemes studied all employed L/G (liquid to gas ratio in absorber) as one quality control variable. Performance comparisons with a typical conventional control scheme are conducted employing a rate-based dynamic model for the MEA (monoethanolamine) solvent PCC process developed on a commercial process simulator. Compared to the typical control scheme, the optimal-based control schemes provide faster responses to the disturbance changes from the flue gas conditions and the set-point change of the CO2 capture efficiency, as well as better results in terms of IAEs (integral of absolute errors) of capture efficiency and reboiler heat duty during the stabilization period. LG-Tstr and LG-Tabs-Cascade are the best schemes. In addition to L/G, these two schemes employ the control of Tstr (the temperature of a stage of stripper) and a cascade control of Tabs (the temperature of a stage of absorber) (outer loop) and Tstr (inner loop), respectively.