As a Quaternary repository of wind-reworked Indus River sand at the entry point in the Himalayan foreland basin, the Thal Desert in northern Pakistan stores mineralogical information useful to trace erosion patterns across the western Himalayan syntaxis and the adjacent orogenic segments that fed detritus into the Indus delta and huge deep-sea fan throughout the Neogene. Provenance analysis of Thal Desert sand was carried out by applying optical and semi-automated Raman spectroscopy on heavy-mineral suites of four eolian and 11 fluvial sand samples collected in selected tributaries draining one specific tectonic domain each in the upper Indus catchment. In each sample, the different types of amphibole, garnet, epidote and pyroxene grains—the four dominant heavy-mineral species in orogenic sediment worldwide—were characterized by SEM-EDS spectroscopy. The chemical composition of 4249 grains was thus determined. Heavy-mineral concentration, the relative proportion of heavy-mineral species, and their minerochemical fingerprints indicate that the Kohistan arc has played the principal role as a source, especially of pyroxene and epidote. Within the western Himalayan syntaxis undergoing rapid exhumation, the Southern Karakorum belt drained by the Hispar River and the Nanga Parbat massif were revealed as important sources of garnet, amphibole, and possibly epidote. Sediment supply from the Greater Himalaya, Lesser Himalaya, and Subhimalaya is dominant only for Punjab tributaries that join the Indus River downstream and do not contribute sand to the Thal Desert. The detailed compositional fingerprint of Thal Desert sand, if contrasted with that of lower course tributaries exclusively draining the Himalaya, provides a semi-actualistic key to be used, in conjunction with complementary provenance datasets and geological information, to reconstruct changes in paleodrainage and unravel the relationship between climatic and tectonic forces that controlled the erosional evolution of the western Himalayan-Karakorum orogen in space and time.