CatVS was applied to two well-known reactions to validate the method: the OsO4-catalyzed cis-dihydroxylation and the Rh-catalyzed asymmetric hydrogenation of enamides. In the former, computational predictions closely matched experimental stereoselectivities, demonstrating the accuracy of the automated setup. In the latter, CatVS was used to screen a library of diphosphine ligands, successfully identifying the most selective candidates.