Exchange of Fe3+ and Fe2+ ions into layers of alpha -zirconium phosphate is achieved in aqueous media by using monosodium and/or ethanolic forms of the host precursor. The products obtained are characterized by chemical analysis, X-ray powder diffraction and Mossbauer spectroscopy. For site assignments, structural modeling is used by combining the measured and simulated X-ray diffractograms. Fe3+ ions are incorporated only in part, and a biphasic product is obtained. Exchange of Fe3+ ions leads to a single phase with 50% iron loading with Fe2+ ions located in two different coordination states. On a long-term storage in open air, Fe-2 divided by --> Fe3+ oxidation proceeds without noticeable change in the crystal structure.