The Lopingian altered volcanic-ash horizons in southwest China have attracted significant attention due to highly-elevated concentrations of critical element Nb-Zr-REY-Ga. Despite extensive investigation, the provenance of these distinctive horizons remains controversial. Are they a product of air-born volcaniclastic, erosional source sedimentation, or a complex mixture of multiple sources?This investigation performs a diverse array of mineralogical and isotopic geochemical analyses to investigate the provenance of these horizons and critical-element mineralization time. The results showed that the concordant ages of detrital zircons 207Pb/206Pb-206Pb/238U from five representative mineralized samples are 253.84 ± 2.60 Ma, 252.49 ± 2.39 Ma, 253.47 ± 2.99 Ma, 257.44 ± 2.01 Ma, and 243.94 ± 2.32 Ma, respectively. Importantly, this dating does not correspond to the stratigraphic position of the studied deposits. Instead, this data set indicates that the low-temperature hydrothermal alteration of the primary Nb-Zr-REY-Ga mineralized layers occurred in Late Permian-Middle Triassic times (260–240 Ma) immediately after volcanic ash deposition at 257–260 Ma. The Sr-Nd-Lu-Hf isotopic compositions, diagrams of both the Al2O3/TiO2 vs. Eu/Eu* and Zr/TiO2 vs. Nb/Y, and the trace element patterns of the zircons (Nb/Hf vs. Th/U, Hf/Th vs. Th/Nb) indicate that the mineralized horizons were derived from both ELIP alkaline rocks and arc-related intermediate-felsic magmatic rocks from the Paleo-Tethys realm. Furthermore, varying amounts of older (∼350 Ma and older) zircon grains defined by the dominant Late Permian-Middle Triassic zircons indicate that there was also some erosional-source input from the uplands surrounding the basin at the time of deposition.