The Greater Caucasus (GC) mountains are the locus of post-Pliocene shortening within the northcentral Arabia-Eurasia collision. Although recent low-temperature thermochronology constrains the timing of orogen formation, the evolution of major structures remains enigmatic—particularly regarding the internal kinematics within this young orogen and the associated Kura Fold-Thrust Belt (KFTB), which flanks its southeastern margin. Here we use a multiproxy provenance analysis to investigate the tectonic history of both the southeastern GC and KFTB by presenting new data from a suite of sandstone samples from the KFTB, including sandstone petrography, whole-rock geochemistry, and detrital zircon (DZ) U-Pb geochronology. To define source terranes for these sediments, we integrate additional new whole-rock geochemical analyses with published DZ results and geological mapping. Our analysis reveals an apparent discrepancy in up-section changes in provenance from the different methods. Sandstone petrography and geochemistry both indicate a systematic up-section evolution from a volcanic and/or volcaniclastic source, presently exposed as a thin strip along the southeastern GC, to what appears similar to an interior GC source. Contrastingly, DZ geochronology suggests less up-section change. We interpret this apparent discrepancy to reflect the onset of sediment recycling within the KFTB, with the exhumation, weathering, and erosion of early thrust sheets in the KFTB resulting in the selective weathering of unstable mineral species that define the volcaniclastic source but left DZ signatures unmodified. Using the timing of sediment recycling and changes in grain size together as proxies for structural initiation of the central KFTB implies that the thrust belt initiated nearly synchronously along strike at ~2.0–2.2 Ma.