With the serious climate change and carbon emissions issues facing the world, it is becoming increasingly important to find effective methods to reduce the post-combustion CO2 concentrations. Piperazine −enhanced aqueous amine solvents are still being developed due to the technology is more applicable to large −scale industry. However, the sustainability of the CO2 capture process is still hindered by high energy consumption and amine losses. To tackle this issue, a novel secondary amine, 2-cyclopentylaminoethanol, was synthesized from a primary amine, monoethanolamine. It has a more stable structure than monoethanolamine and was further activated by piperazine. Its effectiveness was compared with piperazine-enhanced N-methyldiethanolamine, N-methyldiethanolamine/triethylenediamine, and 2-amino-2-methyl-1-propanol. The experimental results showed that 2-cyclopentylaminoethanol/piperazine presents the fastest CO2 mass transfer rate, the largest CO2 cyclic capacity and a lower latent heat. The regeneration energy consumption of the absorbent is approximately 2.44 GJ/ton CO2, which is approximately 37.45% lower than that of 30 wt% monoethanolamine solvent. The results are in accordance with the findings of a laboratory-scale pilot plant study, which demonstrated an average reduction of 35.3% in energy consumption. Molecular simulations have revealed that 2-cyclopentylaminoethanol exhibits the lowest energy barrier for reacting with CO2, rendering it more conducive to CO2 reaction. The intermolecular interactions indicate that the hydrogen bonding in the solution after monoethanolamine reacts with CO₂ becomes more pronounced, coupled with a higher energy barrier. Consequently, a greater amount of energy is required during desorption. It can be inferred that 2-cyclopentylaminoethanol/piperazine is a promising energy-efficient and stable absorbent for post-combustion CO2 capture.