The direct hydrothermal synthesis of Fe-KIT-6 mesoporous materials with Ia3d symmetry and high iron loadings is reported for the first time. The Fe-KIT-6 mesoporous materials were characterized by XRD, N-2 adsorption/desorption isotherms, SEM, FT-IR, XPS and EPR spectroscopy. The physico-chemical characterization results show that all of the samples have well-ordered cubic mesostructures and that the structural integrity is preserved for n(Si)/n(Fe) ratios as high as 10. It was found that most of the iron ions exist as isolated framework species, but for Fe-KIT-6 with an n(Si)/n(Fe) ratio of 10, the presence of extra-framework species/small iron oxide clusters cannot be excluded. The catalytic performances of these materials were tested for carbon dioxide (CO2) hydrogenation and methylcyclopentane (MCP) conversion. The catalytic results show that their catalytic activity increases significantly with increasing iron content. For the MCP conversion, the ring-opening selectivity can be improved by increasing the density of isolated iron atom sites at low reaction temperatures. For the CO2 hydrogenation, the methanation selectivity can be improved by increasing the iron active site density and employing a high reaction temperature. Specifically, the high density of iron sites at high catalyst loadings promotes the methanation reaction at the expense of the RWGS (reverse water gas shift) reaction. Thus, the Fe-KIT-6 materials appear to be suitable catalysts for MCP conversion at low temperatures and CO2 hydrogenation at high temperatures. (C) 2015 Elsevier B.V. All rights reserved.