The PAH101 dataset is available via the NOvel MAterials Discovery (NOMAD) repository and can be accessed at DOI: 10.17172/NOMAD/2024.12.05-1. The data are provided in YAML (.yaml) format. Each file is named as CSD-REFERENCE.archive.yaml, where CSD-REFERENCE is the CSD reference code for each structure. The data structure for each material record is described in Table . The top level sections are struct_id, geometry, dft, and gwbse. The struct_id section contains the CSD reference code. The geometry section provides the fully relaxed crystal structure and the single molecule geometry extracted from it. The dft section contains all the SISSO primary features used in Ref. . The gwbse section provides quasi-particle (QP) and excitonic properties for the PAH101 crystals, including the fundamental gap, quasiparticle band structure, the static dielectric constant, the first singlet exciton energy (optical gap), the first triplet exciton energy, the full dielectric function, and optical absorption spectra for light polarized along the three lattice vectors. The GW static dielectric constant is not available for some of the materials in the dataset because some data that was not needed for Ref. was not preserved. To verify the results of full unit cell relaxation with PBE+TS, the root-mean square distance (RMSD) between the relaxed structures and the experimental structures was calculated. We used the COMPACK 129 molecular overlay method, implemented as the Crystal Packing Similarity tool, in Mercury 2023.2.0 130 . COMPACK overlays clusters of molecules taken from each crystal, within given distance and angle tolerances, and minimizes the RMSD between atoms, typically excluding hydrogen.