Dataset title: Optimization of signal enhancement by photo-CIDNP hyperpolarization with an autosampler compatible NMR probehead Authors: Maria Masik (a,b), Katarzyna Dziubinska-Kuehn (a), Kalle Tiismaa (a), Jaan Past (a), M. Victoria Gomez (c) and Indrek Reile* (a) (a) National Institute of Chemical Physics and Biophysics, Akadeemia tee 23, 12618 Tallinn, Estonia. (b) School of Natural Sciences and Health, Tallinn University, Narva mnt 29, 10120 Tallinn, Estonia. (c) IRICA, Department of Inorganic, Organic and Biochemistry, Faculty of Chemical Sciences and Technologies, Universidad de Castilla-La Mancha (UCLM), Av. Camilo José Cela 10, 13071 Ciudad Real, Spain. *Corresponding author email address: indrek.reile@kbfi.ee The purpose of the dataset is to support the manuscript "Optimization of signal enhancement by photo-CIDNP hyperpolarization with an autosampler compatible NMR probehead" with raw NMR data and extra supporting information. NMR_data: contains raw spectra and the metadata .xlsx and .csv files. fidadd_modified: the modified fidadd macro for Bruker TopSpin. Funding. We acknowledge financial support from the Development Fund on the National Institute of Chemical Physics and Biophysics. NMR experiments were conducted on instrumentation in the Estonian Centre of Analytical Chemistry (AKKI, TARISTU24-TK15). Financial support was obtained from the Estonian Research Council grant MOB3JD1244. M.V.G. thanks the grant PID2023-152323NB-I00 funded by MICIU/AEI/ 10.13039/501100011033 and by ERDF/EU and the grant SBPLY/24/180225/000133 funded by the European Union through European Regional Development Fund (FEDER) and by Junta de Comunidades de Castilla-La Mancha through Castilla-La Mancha Agency for Research and Innovation (INNOCAM). Licence. 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/.