Despite the high-grade diagenesis experienced by the Skoorsteenberg Formation mudstones, Tanqua Karoo basin, South Africa, geochemical data have been interpreted to reveal primary mineralogy and so help understand provenance evolution. The geochemical signatures show systematic variations related to stratigraphy. The main changes in mudstones from the lower to the upper part of the section include: (1) an increase in the feldspar content of the primary sediment and a decrease in the content of Al-rich clay (probably dioctahedral smectite); (2) a decrease in the degree of chemical weathering of the sediment, representing a change to a dryer and/or cooler climate; (3) an increase in TiO2/Al2O3 representing increasing mafic sources; (4) an increase in CaO/(K2O+CaO) also possibly representing increasing mafic sources. Mass flux and differential diagenesis are unlikely to be responsible for the depth-related changes since the rocks have undergone the same degree of high-grade diagenesis and the mudstones are interrupted by other lithologies, so disturbing any sort of diffusion gradient. These variations could plausibly be the result of one or more of differential weathering, evolving provenance characteristics or variable hydrodynamic fractionation of the sediment. The ratio of Zr/Y, a possible indicator of hydrodynamic fractionation, increases only slightly and irregularly up-section. There is no relationship between the silica content, representative of the quartz-silt content of the sediment, and TiO2/Al2O3 showing that the amount of quartz, and so the degree of hydrodynamic fractionation, has not controlled mudstone geochemistry. The stratigraphic increase in feldspar content, the decrease in Al-rich clay content and increase of both TiO2/Al2O3 and CaO/(K2O+CaO) must be due to a combination of marginally evolving provenance characteristics (more mafic and felsic rocks exposed to weathering with time) and changes in the degree of rock weathering (less chemical weathering with time).