This dataset contains raw data used in the manuscript "Combining double-hybrid functionals with rSCAN yields solid-state 13C chemical shifts with sub-ppm accuracy". The dataset contains solid-state NMR spectra, powder X-ray diffraction patterns, crystal structures used in the analysis, and calculated chemical shifts and molecular extractions from CASTEP and Gaussian density functional theory calculations. The data is in various formats and can be viewed using proprietary and free software - more details are given in the Readme file. This work forms part of an undergraduate final year project carried out by the lead author.