CO₂ separation plays an important role in energy saving and CO₂ emission reduction, both of which are necessary to address the issue of global warming. Ionic liquids (ILs) have been proposed to be “green” solvents for CO₂ separation. Unfortunately, the high cost, toxicity, and poor biodegradability of these compounds limit their large-scale application. Deep eutectic solvents (DESs) were recently considered a new type of IL with additional advantages in terms of cost, environmental impact, and synthesis. DESs based on choline salts (i.e., choline-based DESs) are promising candidates for CO₂ separation. In this work, the microstructures, physicochemical properties, and water effect of choline-based DESs are surveyed and compared with those of conventional ILs. The properties of choline-based DESs are similar to those of conventional ILs, but research on the latter remains limited. Further study on the microstructures, properties, and separation performance of choline-based DESs considering dynamic factors must be carried out through experimental measurements and model development. Thermodynamic analysis based on Gibbs free energy change is conducted to investigate the performances of choline-based-DESs during CO₂ separation from biogas. Choline-based-DESs are screened on the basis of energy use and amount of absorbent needed. The performances of the screened choline-based-DESs are further compared with those of conventional ILs screened in our previous work, as well as commercial CO₂ absorbents. Comparisons indicate that the screened DES-based absorbents show great application potential due to their nonvolatility, low energy use, or low amount required. The performances of physical choline-based-DES and 30 wt% MEA for CO₂ separation from other gas streams (e.g., flue gas, lime kiln gas, and bio-syngas) are discussed. Considering the high amounts of physical absorbents required to enable separation, further study with techno-economic analysis needs to be carried out.