Raw NMR data to support and describe the optimization and use of an experimental photo-CIDNP NMR probe, collected on a 300 MHz Bruker Avance III HD spectrometer, equipped with the photo-CIDNP NMR probe. The metadata file is available both as a CSV and XLSX file and describes each raw NMR experiment. The dataset also contains a modified au macro script for Bruker Topspin that was used in data analysis. This dataset is licensed under the Creative Commons Attribution-NonCommercial 4.0 International Licence. A copy of this licence is available at https://creativecommons.org/licenses/by-nc/4.0/.