Binary solvent mixtures based on 1-ethyl-3-methylimidazolium 2-cyanopyrrolide, , an ionic liquid (IL), and a series of hydrogen bond donors (HBDs) including ethylene glycol (EG), propylene glycol (PG), and monoethanolamine (MEA) were characterized in terms of temperature-dependent densities and viscosities along with their thermal stability and CO 2 absorption−desorption capability. NMR and FTIR were employed to observe the effect of the IL/HBD composition on intermolecular interactions. Among the investigated mixtures, IL/EG (1:2) showed the most efficient absorption−desorption performance and thermal stability. Though IL/PG and IL/EG had similar CO 2 absorption capacities, the IL/PG exhibited the highest viscosity, which limited the CO 2 transport in the solvent. The IL/MEA solvent possesses significant CO 2 absorbance capability; however, the strong binding energy between MEA and CO 2 and the increased viscosity during absorption led to difficulties in CO 2 desorption. This study highlights the modification of intermolecular interactions in IL/HBD binary mixtures with respect to the choice of HBDs, reflected by their distinct physical properties and CO 2 binding behavior.