The supporting information is available free of charge.Grazing incidence X-ray diffraction patterns (GIXRD) of the [{Mo 6 I i 8 }I a 4 (H 2 O) a 2 ].xH 2 O photoelectrode, XPS analyses (wide-range spectra, I 3d, Mo 3d and Cs 4d) obtained on the MC film and the MC precursor powder and charge carrier lifetimes determined on the MC film via the OCP decay (file type, i.e., PDF).