This dataset provides supporting research data for the study of molecular rotation and large polarization in charge-transfer cocrystal ferroelectrics. It contains a compressed archive of electronic structure calculations and spreadsheet files with source data for several reported figures, including Figure 2, Figure 3, and Figure 4E. The data are intended to support analysis and reproduction of computational and plotted results related to ferroelectric behavior, charge-transfer cocrystal properties, molecular rotational mechanisms, and polarization responses in these materials.