Accordingly (Fig. ) we developed a dataset of 8,000 DFT optimized structures with ca. 200,000 DFT computed chemical shifts (the DFT8K dataset). All datasets generated by this work are shared openly. We began by sampling a subset of structures from the NMRShiftDB, which contains 43,475 structures at the time of writing. The sampling procedure is as follows: we first extracted all neutral organic molecules with MW < 500. From the resulting set of around 20,000 structures, 8,000 were selected by a farthestneighbor algorithm to create a computationally manageable dataset while maximizing structural diversity.