The dataset was further enriched by molecules with previously published CSP and experimental results with relevance to small-molecule pharmaceuticals. The final dataset, comprising 66 molecules, covers a diversity of functional groups, including polar groups such as amide, urea, pyridine, sulfonamide, hydroxyl, nitro, carboxylate, cyano, nonpolar groups such as phenyl and alkane chains, and various substituted aromatic and nonaromatic rings. The functional group diversity present in the dataset requires high accuracy of the energy models across chemical space, particularly as it applies to intra-and inter-molecular interactions relevant for molecular crystal packing.