Aggregation affects a wide range of physical and biogeochemical soil properties with positive effects on soil carbon storage. For weathered tropical soils, aluminous clays (kaolinite and gibbsite) and pedogenic Fe (oxyhydr)oxides (goethite and hematite; termed "Fe oxides") have been suggested as important building units for aggregates. However, as aluminosilicates, aluminum hydroxides, and Fe oxides are part of the clay-sized fraction it is hard to separate how certain mineral phases modulate aggregation. In addition, it is not known what consequences this will have for organic carbon (OC) persistence after land-use change. We selected topsoils with unique mineralogical compositions in the East Usambara Mountains of Tanzania under forest and cropland land uses, varying in contents of aluminous clay and Fe oxides. Across the mineralogical combinations, we determined the aggregate size distribution, aggregate stability, OC contents of aggregate size fractions, and changes in aggregation and OC contents under forest and cropland land use. Patterns in soil aggregation were rather similar across the different mineralogical combinations (high level of macroaggregation and high aggregate stability). Nevertheless, we found some statistically significant effects of aluminous clay and pedogenic Fe oxides on aggregation and OC storage. An aluminous clay content >g250gkg-1 in combination with pedogenic Fe contents <g60gkg-1 significantly promoted the formation of large macroaggregates >g4gmm. In contrast, a pedogenic Fe content >g60gkg-1 in combination with aluminous clay content of <g250gkg-1 promoted OC storage and persistence even under agricultural use. The combination with low aluminous clay and high pedogenic Fe contents displayed the highest OC persistence, despite conversion of forest to cropland causing substantial disaggregation. This indicates that aggregation in these tropical soils is modulated by the mineralogical regime, causing moderate but significant differences in aggregate size distribution. Nevertheless, aggregation was little decisive for overall OC persistence in these highly weathered soils, where OC storage is more regulated by direct mineral-organic interactions.