The integration of ICP-OES, XRD, chemical analysis, and scanning electron microscopy was used to investigate the source area, weathering, paleoclimate conditions, and provenance of the siltstones of the Santa Maria Formation (Middle to Upper Triassic, Southern Brazil). This unit is regionally subdivided, from base to top, into the Passo das Tropas Member (Late Anisian–Middle Ladinian) and the Alemoa Member (Middle Ladinian–Carnian). The Chemical Index of Alteration (CIA) was calculated for both members to highlight the weathering processes of primary minerals. The CIA results indicate moderate to extreme weathering of the source rocks for the siltstones. The extreme chemical alteration observed in the Passo das Tropas siltstones (CIA = 76.97–90.83) and in the mid-section of the Alemoa Member (CIA = 87.96–89.63) suggests weathering under more humid conditions, related to an increase in paleorainfall. Paleoclimate was interpreted as semi-arid to arid, with alternating wet and dry seasons. These results align with the geochemical behavior of uranium and thorium. Samples with higher CIA values show higher Th/U ratios, indicating a shift toward a more humid climate. X-ray diffraction analysis of the fine fraction (FF < 2 μm) of the samples identified mixed-layered illite-smectite (I/S) clay minerals with minor amounts of quartz. Regarding provenance, Th/U ratios coupled with Th vs. Sc and La-Th-Sc plots, suggest an upper crustal protolith for the southern Santa Maria siltstones, consisting of uplifted rocks from the crystalline basement of the Sul-Rio-Grandense shield and sedimentary rocks of the Camaquã Basin. The Th/Sc, Sc/Th, Co/Th, and La/Sc ratios, along with the contents of Al₂O₃, SiO₂, TiO₂, Co, V, Ni, and Sc, indicate a more felsic composition for the Passo das Tropas Member. Meanwhile, the source rocks of the Alemoa Member sediments demonstrate a more mafic composition in the mid-section, transitioning to a felsic composition in the uppermost succession.