This paper presents a detailed sedimentologic investigation of a newly identified, fossiliferous Late Neogene sedimentary succession in the Rukwa Rift Basin, southwestern Tanzania. This synrift deposit is a rare and significant new example of a fossiliferous succession of this age in the Western Branch of East Africa Rift System. The unit, informally termed the lower Lake Beds succession, is late Miocene to Pliocene in age based on cross-cutting relationships, preliminary biostratigraphy, and U-Pb geochronology. An angular unconformity separates the lower Lake Beds from underlying Cretaceous and Oligocene strata. Deposition was controlled by rapid generation of accommodation space and increased sediment supply associated with late Cenozoic tectonic reactivation of the Rukwa Rift and synchronous initiation of the Rungwe Volcanic Centre. The lower Lake Beds, which have thus far only been identified in three localities throughout the Rukwa Rift Basin, are characterized by two discrete lithologic members (herein A and B). The lower Member A is a volcanic-rich succession composed mostly of devitrified volcanic tuffs, and volcaniclastic mudstones and sandstones with minor conglomerates. The upper Member B is a siliciclastic-dominated succession of conglomerates, sandstones, mudstones and minor volcanic tuffs. Detailed facies analysis of the lower Lake Beds reveals various distinctive depositional environments that can be grouped into three categories: 1) alluvial fan; 2) fluvial channel; and 3) flood basin environments, characterized by volcanoclastic-filled lakes and ponds, abandoned channel-fills and pedogenically modified floodplains. Member A represents a shallow lacustrine setting filled by tuffaceous sediments, which grade up into a system of alluvial fans and high-energy, proximal gravel-bed braided rivers. An unconformity marks the contact between the two members. Member B shows an upward transition from a high-energy, gravel-bed braided river system to a sandy braided river system with increasingly abundant floodplain deposits and well-developed paleosols. Vertebrate fossils are sparse in member A, but common in member B, preserved both within pedogenic soil horizons and as isolated elements and microsites within fluvial channel facies associations. Faunal remains include fishes, turtles and crocodylians, along with well-preserved mammal cranial and post-cranial remains. In addition, freshwater gastropod shells are locally present in member A and continental trace fossils, including abundant fossilized termite nests, are present in both members.