The uniform corrosion rate of oxide-covered iron increases under illumination. This dataset contains measurements associated with an investigation of the mechanism of this increase. The samples were polished iron samples. Polished iron was either investigated directly, or anodised to create oxide films with thicknesses of 50-350 nm. The dataset contains the following experimental results: (i) potentiodynamic polarisation curves of polished iron in different electrolytes (acid, neutral, chloride-containing, alkaline) with and without white light illumination; (ii) potentiodynamic polarisation curves of anodised iron with different oxide thicknesses in NaOH with and without white light illumination; (iii) potentiodynamic polarisation curves of anodised iron in NaOH with monochromatic illumination (450-800 nm wavelength); (iv) photocurrent and photovoltage transients of polished and anodised iron in NaOH under different illumination and polarisation conditions; and (v) ex situ UV-VIS spectra of anodised iron with different oxide thickness vs. an aluminium reference. All polarisation curves were measured under controlled convection, which enabled a quantification of different contributions to the overall uniform photocorrosion rate of iron. The dataset contains ASCII files with descriptive filenames and is structured in subfolders indicating the respective methods. A detailed interpretation of the results, and the experimental details associated with the dataset is available in the associated article.