Dataset description Hybrid magneto-molecular devices are ideal systems to design multifunctional devices in which optical and spin properties are interlinked. In the paper, Optical Conversion of Pure Spin Currents in Hybrid Molecular Devices we give an account of how the propagation of pure spin currents into molecular layers, in particular C60, results in changes to the optical absorbance, Raman spectrum and luminescence of the fullerene. We also show that optical irradiation in these compounds can lead to an enhanced spin mixing conductance. This dataset contains the data for the results in the manuscript. All the files presented in this dataset are Origin files and can be opened using Origin viewer software accessed at: • http://www.originlab.com/viewer/ • http://www.originlab.com/viewer/dl.aspx