Sedimentological, provenance, and detrital thermochronological results for basin fill at the modern deformation front of the northern Andes (6°N latitude) provide a long-term, Eocene to Pliocene record of foreland-basin sedimentation along the Eastern Cordillera–Llanos basin boundary in Colombia. Lithofacies assemblages and paleocurrent orientations in the upward-coarsening, ~5-km-thick succession of the Nunchía syncline reveal a systematic shift from craton-derived, shallow-marine distal foreland (back-bulge) accumulation in the Mirador Formation, to orogen-sourced, deltaic, and coastal-influenced sedimentation of the distal to medial foreland (foredeep) in the Carbonera and León Formations, to anastomosing fluvial and distributive braided fluvial megafan systems of the proximal foreland (foredeep to wedge-top) basin in the lower and upper Guayabo Formation. These changes in depositional processes and sediment dispersal are supported by up-section variations in detrital zircon U-Pb and (U-Th)/He ages that record exhumation of evolving, compartmentalized sediment source areas in the Eastern Cordillera. The data are interpreted in terms of a progressive eastward advance in fold-and-thrust deformation, with late Eocene–Oligocene deformation in the axial zone of the Eastern Cordillera along the western edge of Floresta basin (Soapaga thrust), early Miocene reactivation (inversion) of the eastern margin of the Mesozoic rift system (Pajarito and Guaicaramo thrusts), and middle–late Miocene propagation of a footwall shortcut fault (Yopal thrust) that created the Nunchía syncline in a wedge-top (piggyback) setting of the eastern foothills along the transition from the Eastern Cordillera to Llanos foreland basin. Collectively, the data presented here for the frontal Eastern Cordillera define a general in-sequence pattern of eastward-advancing fold-and-thrust deformation during Cenozoic east-west shortening in the Colombian Andes.