The origin of large and small particle axial bands in long rotating tumblers is a long-standing question. Using DEM simulations, we show that this axial segregation is due to a Rayleigh-Taylor instability which is characterized by the fact that the density of a granular medium increases with mixing and decreases with segregation. For initially mixed particles, segregation and collisional diffusion in the flowing layer balance and lead to a three-layer system, with a layer of large particles over a layer of small particles, and, interposed between these layers, a layer of more densely packed mixed particles. The higher density mixed particle layer over the lower density small particle layer induces a Rayleigh-Taylor instability, evident as waviness in the interface between the layers. The waviness destabilizes into ascending plumes of small particles and descending plumes of mixed particles with large particles enriched near the surface, which become evident as small and large particle bands visible at the free surface. Rolls driven by segregation at the tilted interface between plumes maintain the pattern of frozen plumes. Published by the American Physical Society 2024