Although some differences in torsional preferences were found, most cases of poor correlation between experimental COD geometries and lowest-energy CREST/GFN2 conformers occur with a lack of sufficient experimental crystallographic data. Some deviations occur from new subpopulations not present in the experimental databases, as not every compound can be crystallized. Using density functional methods to optimize compounds in such subpopulations, we find torsion angle deviations ∼0-5 • , suggesting CREST/GFN2 to be sufficiently accurate for generating overall torsion angle distributions, even if some errors remain.