Chemical hydrogen storage and release of iron-based oxide mediums were investigated by hydrogen reduction and water splitting oxidation (Fe3O4 + 4H2 ⇌ 3Fe + 4H2O). In this study, all metal oxide mediums were prepared by coprecipitation method using urea solution as precipitant. The redox reactions of the mediums were conducted using a fixed bed quartz reactor under atmospheric pressure. The theoretical amount of hydrogen storage that can be obtained from the redox reaction of iron oxide is calculated to be 4.8wt% on the basis of 1g-Fe. However, in case of using the iron oxide medium without additives, the medium was rapidly deactivated due to the agglomeration of Fe metals in the hydrogen reduction step of repeated redox cycles. In this study, therefore, Mo and Zr additives were added to iron oxide to improve the reactivity of the medium and to prevent the agglomeration of that. As a result, the reactivity for oxidation of the mediums was largely improved with the addition of Mo additive. It was concluded that change in the valence of Mo cations affected the redox behavior of the mediums.