Heat-duty reduction is the major challenge in CO2 desorption and amine regeneration. The use of a combination of heterogeneous catalytic desorption with improved amine solvents is a novel approach to address this issue. We studied CO2-desorption tests of noncatalytic diethylamine (DEA) solvents as a benchmark and focused on five blended amines (DEA-monoethanolamine, MEA; 4.5:0.5 to 2.5:2.5 M) with three types of catalysts (gamma-Al2O3, H-ZSM-5, and 2:1 blended gamma-Al2O3 H-ZSM-5) to explore the synergy effects of DEA-based amine blends with solid catalysts. The heat duty and CO2 production of each case scenario were tested for six sets of solutions with initial loading of 0.5 mol of CO2 per mole of amine at 363-378 K and were compared with those of 5 M DEA solvents. The results showed that the three catalyst conditions (blended catalyst, H-ZSM-5, and gamma-Al2O3) followed different trends at rich and lean loadings. Finally, both 5 M DEA and 4.5:0.5 M DEA MEA with blended catalysts exhibited very low heat duties of 151.2 and 168.0 kJ per mole of CO2 at loadings of 0.50-0.20 mol per mole of amine at 378 K among the six solutions. Both approaches proved to be the most-energy-efficient amine solutions whereas the blended amine with blended catalysts was the best strategy that was applicable in the CO2 desorber.