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Integration of sequence stratigraphy, magnetostratigraphy, Ar/Ar dating, and paleontology considerably advances knowledge of the Late Cretaceous-early Paleogene chronostratigraphy and tectonic evolution of Bolivia and adjacent areas. The partly restricted marine EI Molino Formation spans the Maastrichtian and Danian (-73-60.0 Ma). Deposition of the alluvial to lacustrine Santa Lucía Formation occurred between 60.0 and 58.2 Ma. The widespread erosional unconformity a t the base of the Cayara Formation is 58.2 Ma. This unconformity separates the Upper Puca and Corocoro supersequences in Bolivia, and is thus coeval with the Zuni-Tejas sequence boundary of North America. The thick overlying Potoco and Camargo formations represent a late Paleocene-Oligocene foreland fill. The onset of shortening along the Pacific margin at-89 Ma initially produced rifting in the distal foreland. Santonian-Campanian eastward-onlapping deposits indicate subsequent waning of tectonic activity along the margin. Significant tectonism and magmatism resumed along the margin a t-73 Ma and produced an abrupt increase in subsidence rate and other related phenomena in the basin. Subsidence was maximum between-71 and-66 Ma. Due to the early Maastrichtian global sea-level high, marine waters ingressed from the northwest into this underfilled basin. Subsidence decreased during the Late Maastrichtian and was low during the Danian. It increased again in the latest Danian, for which a slight transgression is recorded, and peaked in the early Selandian. Tectonism between 59.5 and 58.2 Ma produced a variety of deformational and sedimentary effects in the basin and correlates with the end of emplacement of the Coastal batholith. The subsequent 58.2 Ma major unconformity marks the onset of continental foreland basin development, which extended into Andean Bolivia during the late Paleocene-Oligocene interval. This basin underwent internal deformation as early as Eocene time in the Altiplano and Cordillera Oriental. These early structures, previously assigned to the late Oligocene-early Miocene orogeny, probably accommodated observed tectonic rotations in the Eocene-Oligocene.