This study investigates the effect of using water as a low-viscosity component in ternary amine-based deep eutectic solvents (DESs) on the physicochemical properties, thermal stability, and CO2absorption capacity of the resulting DESs. It should be emphasized that water is a component of the ternary DES. The effect of water content in the DES, type of hydrogen bond acceptors (HBAs), hydrogen bond donors (HBDs), and HBA:HBD ratio on the above parameters was investigated. Moreover, the effect of temperature and pressure on the CO2absorption capacity of DESs was predicted using the predictive model COSMO-RS. This model was also used to predict the CO2solubility in the DESs and the results were compared with the experimental values. The results showed that the addition of small amounts of water, e.g., 5 and 10 wt% during preparation, can significantly decrease the viscosity of the resulting DESs, up to 25% at room temperature, while maintaining the high CO2absorption capacity and high thermal stability. The ternary DESs based on MEA exhibited a high CO2absorption capacity of 0.155–0.170 g CO2/ g DES. The ternary DESs were found to be thermally stable with a decomposition temperature of 125°C, which promotes the use of such solvents in post-combustion capture processes. Finally, COSMO-RS proved to be a suitable tool for qualitative prediction of CO2solubility in DESs and demonstration of trends related to the effects of temperature, pressure, molar ratio, water content, HBD and HBA on CO2solubility.