A modified red mud-(MRM-) supported Fe catalyst ( Fe/MRM) was prepared using the homogeneous precipitation method and applied to methane decomposition to produce hydrogen. The TEM and SEM-EDX results suggested that the particle sizes of the Fe/MRM catalysts were much smaller than that of raw red mud (RM), and the active metal Fe was evenly distributed over the catalyst structure. Moreover, BET results indicated that the surface areas and pore volumes of the catalysts were significantly improved, and the pore sizes of Fe/MRM were distributed from 5 to 12 nm, which is typical for a mesoporous material. The activities of those catalysts for the catalytic decomposition of methane were studied at atmospheric pressure at a moderate temperature of 650 ∘ C; the results showed that the Fe/MRM catalysts were more active than RM and MRM. The methane conversion curves of Fe/MRM catalysts exhibited similar variation tendencies (three-step) during the reaction despite different Fe contents, and the loading amount of Fe clearly affected the activity of the catalysts.