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Amine-based postcombustion CO2 capture technology has a great potential to control CO2 emissions but is expensive because a huge amount of thermal energy is required for solvent regeneration due to poor CO2 desorption kinetics. Tertiary amines can be efficiently regenerated, but the poor CO2 absorption kinetics are a major limitation to its large-scale deployment. Here, we synthesized tripodal nitrate salt and its metal catalysts and investigated catalytic activity in a highly concentrated tertiary amine medium, N-methyldiethanolamine (MDEA), for the CO2 capture process. To analyze the catalytic performance, the rate constant for CO2 hydration, CO2 absorption rate, and CO2 desorption rate were experimentally studied. The gathered results suggest that catalyst 2 can improve the CO2 absorption and CO2 desorption efficiencies by 35% and 21%, respectively. On the basis of the obtained results, the possible reaction mechanism is also presented. These findings can provide a new route for energy-efficient CO2 capture using tertiary amines.