The data records include the DFT primary features used for SISSO in Ref. . The DFT features of molecules and crystals were calculated using FHI-aims . From considerations of computational efficiency, the DFT primary features were calculated with locally-optimized geometries. The crystal structures were relaxed with the lattice vectors fixed at the experimental values and the single molecule properties were calculated using molecules extracted from these locally-optimized crystal structures. All primary features were calculated with the PBE functional. 121 using the tight numerical setting and tier-2 basis sets of FHI-aims. 119