The upper Oligocene to lower Miocene Peñas and Aranjuez formations are exposed in north-northwest–trending outcrop belts of the central Andean backthrust belt situated within the central Andean plateau along the boundary between the northern Altiplano and the Eastern Cordillera of Bolivia. Sedimentary lithofacies analyses indicate that these coarse-grained siliciclastic formations were deposited primarily in alluvial fan to braided fluvial environments. An upsection change from principally fine-grained sandstone to cobble conglomerate is consistent with increased proximity to the sediment source with time. Paleocurrent analyses reveal that flow was predominantly directed toward the west-southwest away from Cordillera Real, the elevated core of the Eastern Cordillera. Provenance data from conglomerate clast compositions and sandstone petrofacies suggest derivation from recycled quartz-rich metasedimentary and sedimentary rocks from the Paleozoic section in the Eastern Cordillera. The paleoflow orientations, sediment provenance, and increased proximity of the sediment source suggest that deposition of the Peñas and Aranjuez formations was related to surface uplift of the Eastern Cordillera relative to the Altiplano. Growth strata observed in the Aranjuez Formation further indicate that shortening was synchronous with deposition, probably in a hinterland basin. New 40Ar/39Ar ages from a lowermost exposed igneous unit and interbedded ash-fall tuff beds in the Aranjuez and Peñas formations show that synorogenic sedimentation and fold-thrust deformation in the frontal (west-southwestern) zone of the central Andean backthrust belt was concentrated during late Oligocene–early Miocene time. These age results are consistent with previous studies of east-derived sedimentation in the Altiplano and indicate regional uplift of the Eastern Cordillera at this time. Upsection trends in provenance data further suggest a progressively greater contribution from younger Paleozoic strata, possibly due to activation of new thrust faults during west-southwestward propagation of the backthrust belt toward the Altiplano. Such a progression of late Oligocene–early Miocene shortening along the Altiplano–Eastern Cordillera boundary likely reflects significant crustal thickening, potential isostatic uplift, and initial topographic expression of the eastern margin of the central Andean plateau.