This dataset contains spectropolarimetric measurements obtained in the 4227A Ca line near the solar limb with the GREGOR telescope in Tenerife and with the Gregory Coudé Telescope at IRSOL in Locarno. The observations are discussed in the article Capozzi, E., Alsina Ballester, E, Belluzzi, L., Bianda, M., Dhara, S.K., Ramelli, R.: 2020, "Observational indications of magneto-optical effects in the scattering polarization wings of the Ca I 4227 A line", Astronomy and Astrophysics, 641, A63, doi:10.1051/0004-6361/202038455, arXiv:2006.13653