Clay minerals and pedogenic metal (oxyhydr)oxides are the most reactive soil mineral constituents controlling the long-term persistence of organic carbon (OC) in terrestrial ecosystems. However, their co-occurrence in most soils complicates direct assessment of their individual contribution to OC persistence. Making use of unique mineralogical combinations in soils located in the East Usambara Mountains of Tanzania, we disentangled the contribution of clay-sized aluminous minerals (kaolinite, gibbsite) and pedogenic Fe (oxyhydr)oxides (predominant goethite and hematite) on OC storage and stabilization under natural forests and croplands. Topsoil samples, varying in contents but not types of aluminous clays and pedogenic Fe (oxyhydr)oxides, were identified by selective extractions, X-ray diffraction, and Mössbauer spectroscopy. Associated abundance of particulate and mineral-associated organic matter (OM) was quantified by density fractionation and their changes during land-use conversion were determined as a measure of OC persistence. Additionally, we assessed the resistance of OC to chemical oxidation as well as microbial decomposition in a 50-day laboratory incubation. We found that the ratio of pedogenic Fe to aluminous clay is more consequential for OC storage and stabilization than their individual contents, despite the fact that Fe (oxyhydr)oxides generally exert a stronger impact on OC than aluminous clays. Conjunction of large amounts of Fe (oxyhydr)oxides with low aluminous clay contents caused the strongest accumulation of mineral-associated OC, a low soil respiration, high OC stability against chemical oxidation, and high OC persistence during land-use change. Our study suggests that certain mineralogical combinations in the humid tropics alleviate OM losses during land conversion because of the strong and selective mineral control on OC stabilization, particular if the weight ratio of pedogenic Fe to aluminous clay exceeds the threshold range of 0.44‒0.56.