The tectonism, volcanism, and sedimentation along the East African Rift System (EARS) produced a series of rift basins with a rich paleoanthropological record, including a Late Miocene–present record of hominin evolution. To better understand the relationship between Earth system history and human evolution within the EARS, the Hominin Sites and Paleolakes Drilling Project (HSPDP) collected paleolake sediments near key paleoanthropological sites in Ethiopia and Kenya, compiling a multi-proxy, high-resolution geological and environmental record. As part of the HSPDP, I studied the detrital mineral record of the basins and evaluated tectonic and climatic controls on East African landscapes during the Plio-Pleistocene using samples from three of the drill sites, Chew Bahir: (CHB, ~620–present; Ethiopia), Northern Awash (NA, ~3.3–2.9 Ma; Ethiopia,), and West Turkana (WTK, ~1.9–1.4 Ma; Kenya). I employed laser ablation U/Pb and (U-Th)/He double dating (LADD) of detrital zircons, which yields paired U/Pb and (U-Th)/He dates, and (U-Th)/He dating of detrital apatites to evaluate sediment provenance and the cooling history of the source rocks. In addition, I used in situ 10Be cosmogenic radionuclide analyses to determine paleoerosion rates. Two chapters of this dissertation focus on results from the NA and WTK drill sites. Source units for the NA and WTK drill sites are largely Cenozoic volcanic rocks, and the detrital zircon record yields an extensive record of the timing of various phases of volcanism within the EARS. Exceptionally young zircon (U-Th)/He dates reflect partial resetting associated with late mafic volcanism and/or hydrothermal activity. Erosion rates are consistent and relatively low across the Plio-Pleistocene, despite significant tectonic and geomorphic shifts in the landscape. Two other chapters of this dissertation cover results from the CHB drill site. The Chew Bahir basin has significant exposures of Neoproterozoic and Early Paleozoic crystalline basement units, and the detrital zircon record yields one singular phase of volcanism in the EARS. The CHB erosion rates show an overall decreasing trend over time, consistent with an aridifying climate, and increased environmental variability after ~200 ka.