This dataset contains (TD-)DFT calculations for a series of N-Tolanyl-phenochalcogenazines PZX in neutral and radical form with two different geometries. For the radicals, only the DFT geometry optimization is given, while for the neutral forms the TD-DFT calculation is given. The dataset is used in a print publication from the Lambert group with the title “Structure and Photophysics of N-Tolanyl-phenochalcogenazines and their Radical Cations”