Fifteen different low molar mass compounds are assessed as CO2 solvents based on bubble-point loci on the solvent-rich end (0.6 to 1.0 solvent wt fraction) of the CO2-solvent pressure-composition diagram at 298.15 K. Four of the five best solvents (in descending order of solvent strength on a mass fraction CO2 dissolved basis), acetone, methyl acetate, 1,4-dioxane, and 2-methoxyethyl acetate, are oxygen-rich, low molar mass species possessing one or more oxygen atoms in carbonyl, ether, and/or acetate groups that can interact favorably with CO2 via Lewis acid/Lewis base interactions. Methanol, a very low molar mass solvent, is comparable to 1,4-dioxane in solvent strength. The remaining solvents, in descending order of solvent strength on a mass basis, include 2-nitropropane, N,N-dimethylacetamide, acetylacetone, 1-nitropropane, iso-octane, 2-(2-butoxyethoxy)ethyl acetate, N-formylmorpholine, propylene carbonate, 2-butoxyethyl acetate, and N-tert-butylformamide. When compared on a molar basis, each of the six best CO2 solvents, 2-(2-butoxyethoxy)ethyl acetate, methyl acetate, 2-methoxyethyl acetate, 1,4-dioxane, acetone, and acetyl acetone, is rich in CO2-philic ether or carbonyl oxygen atoms. Methanol, which possesses a CO2-phobic hydroxyl group, is the worst CO2 solvent. COSMOtherm accurately predicted the relative solvent strengths of eight of the solvents that contain carbonyl, acetate, ether, and carbonate groups. However, COSMOtherm was not able to predict the correct ordering of solvents possessing hydroxyl, nitro-, amide, secondary amine, and tertiary amine groups. This important failure of the COSMOtherm approach for these molecules is apparently due to problems with the COSMO-RS parametrization.