The COnductor-like Screening MOdels-Segment Aactivity Coefficient (COSMO-SAC) is a promising approach for computing activity coefficients in the liquid phase. Using Deep Eutectic Solvents (DESs) as green solvents to absorb greenhouse gases, particularly carbon dioxide (CO2), has attracted noticeable attention in research. Despite this, few modeling investigations have employed the COSMO-SAC model for estimating carbon dioxide solubility in choline chloride-based DESs. Our research aimed to overcome the obstacles with group contribution methods’ parameters using the COSMO-SAC model which employs general parameters. In our study, we developed and validated the model using around 80% of the datasets, with the remaining 20% used for testing. The range of average relative deviation varied between 7.64% to 47.84. Furthermore, the calculation results indicated decreased average relative deviations at lower temperatures. The findings exhibited that the model is qualitatively successful in predicting carbon dioxide solubility in choline chloride-based DESs. However, adding more solvents and experimental data to enhance the model’s accuracy would broaden the model’s applicability to various DESs.