Recent studies indicate that mantle plumes, which transfer material and heat from the earth’s interior to its surface, represent multifaceted upwellings. The Tristan-Gough hotspot track (South Atlantic), which formed above a mantle plume, documents spatial geochemical zonation in two distinct sub-tracks since ~70 Ma. The origin and the sudden appearance of two distinct geochemical flavors is enigmatic, but could provide insights into the structural evolution of mantle plumes. Sr–Nd–Pb–Hf isotope data from the Late Cretaceous Rio Grande Rise and adjacent Jean Charcot Seamount Chain (South American Plate), which represent the counterpart of the older Tristan-Gough volcanic track (African Plate), extends the bilateral-zonation to ~100 Ma. Our results support recent numerical models, demonstrating that mantle plumes can split into distinct upper mantle conduits, and provide evidence that these plumelets formed at the plume head-to-plume tail transition. We attribute the plume zonation to sampling the geochemically-graded margin of the African Large Low-Shear-Velocity Province.