Utilization of ionic liquids (ILs) for carbon dioxide (CO2) capture is continuously growing, and further understanding of the factors that influence its solubility (notably for new ILs) is crucial. Herein, CO2 absorption of two 1,2,4-triazolium-based ILs was compared with imidazolium-based Ils of different anions, namely bis(trifluoromethylsulfonyl)imide, tetrafluoroborate, and glycinate. The CO2 absorption capacity was determined using an isochoric saturation method and compared with predicted solubility employing COnductor-like Screening Model for Real Solvents (COSMO-RS). To gain an understanding of the effects of cations and anions of the ILs on the CO2 solubility, the molecular orbitals energy levels were calculated using TURBOMOLE. Triazolium-based ILs exhibit higher absorption capacity when compared to imidazolium-based ILs for the same anions. The results also showed that the anions� energy levels are more determinant towards solubility than the cations� energy levels, which can be explained by the higher tendency of CO2 to accept electrons than to donate them. © 2023 by the authors.