The Mbarga itabirite deposit in the Mbalam iron district on the northwest edge of the Congo Craton (CC) hosts two main types of iron ore enrichments: supergene and specularite ores. This study presents mineralogical, geochemical, and isotopic datasets on these ores to determine their genesis.Ore microscopic studies indicate that the itabirites are of the oxide facies type, with magnetite showing partial to extensive alteration to hematite-martite. The supergene ores consist of hematite + martite + goethite ± gibbsite ± magnetite ± quartz, while the specularite ores are mainly composed of hematite + martite ± quartz. Magnetite microchemistry suggests formation under low-T hydrothermal conditions (~200–300 °C) with high fO2. Geochemical analyses show that the supergene and specularite ores have higher Fe2O3 (88.27 to ~100 wt%) and lower SiO2 (<0.01 to 0.18 wt%) contents than the itabirites (31.95 wt% Fe2O3, 67.16 wt% SiO2). The enrichment of Fe in the supergene ores is attributed to the depletion of major oxides and trace elements due to weathering and supergene enrichment, while the high Fe content in the specularite ores stems from the precipitation of iron-rich, but trace- and rare earth elements (REE)-deficient hydrothermal fluids. The slightly higher Al2O3 content and positive Ce anomalies in the supergene ores suggest the retention of Al-bearing minerals (gibbsite) and reveal highly oxidative conditions during martitization. Stable isotope analyses reveal that the supergene and specularite ores have δ18O values of −2.5 to −0.3 ‰ and − 2.0 to −3.4 ‰, and δ2H values of −75 to −123 ‰ and − 70 to −119 ‰, respectively, suggesting the involvement of isotopically light-evolved meteoric water in their formation. In contrast, the itabirites exhibit heavier δ18O (8.5 to 10.2 ‰) and δ2H (−85 to −91 ‰) values, suggesting formation from mixed magmatic and metamorphic fluid sources. A “polygenic-supergene-hydrothermal” model is suggested for the formation of the Mbarga itabirite-hosted iron ores.