Two iron deposits within the Precambrian mineral belt of Cameroon are described in detail for the first time: the Archean Metzimevin replacement iron deposit enclosed in Fe-enriched itabirite, and the Proterozoic granite-hosted, shear zone-related Mayo Binka magnetite deposit. In the Metzimevin deposit, quartz is corroded and microplaty hematite overprints martite-textured hematite. The Mayo Binka massive magnetite veins show evidence of deformation in magnetite (fracturing and microbrecciation) and in overgrowths of specular hematite (mechanical twinning and undulating extinction). The magnetite is partially replaced by hematite (martitization) and goethite. Ores from both deposits have >88% total Fe2O3 and low contents of contaminants such as SiO2, Al2O3, MgO, CaO, P2O5, and TiO2. They are also poor in Cu, Pb, Zn, V, Cr, and Ni. The Metzimevin massive hematite is characterized by an accentuated light rare earth element depletion relative to the Fe-enriched itabirite. It is suggested that the Metzimevin iron deposit is the result of hypogene leaching of gangue minerals from, and further hematitization of, an itabirite protore. Although the genesis of the Mayo Binka massive magnetite is unclear, it is spatially related to Neoproterozoic granitic rocks. The data allow some comparison of these little known, but potentially economic iron deposits, with some of the world’s better investigated deposits, and are useful to the exploration efforts for iron ore currently underway in Cameroon and the Central African subregion.