In this study, we present the first high-resolution data from coupled δ 34 S analyses of carbonate-associated sulfate (CAS) and chromium-reducible sulfur (CRS) from three Lower–Middle Cambrian sections in western Gondwana. CAS and CRS were extracted and analyzed from marine dolostone, limestone, and nodular limestone from Spanish and French successions. In parallel, carbonate samples were also analyzed for δ 13 C carb , δ 18 O carb , and major/trace element concentrations (Ca, Fe, Mg, Mn, Sr). δ 34 S CAS values vary between 17.6‰ and 33.2‰, with a maximum CAS concentration of ca. 900ppm. δ 34 S CRS data show a similar broad range between −5.1‰ and 29.7‰, with maximal CRS contents up to ca. 3700ppm. Notably, there is little stratigraphic variation in the δ 34 S CAS data in each of the sections confounding inter-basinal chemostratigraphic correlations. Nonetheless, the absolute differences in δ 34 S CAS between sections as well as variations in CAS and CRS concentrations are attributed to paleoenvironmental differences between proximal and distal parts of the carbonate ramp, as well as effects of subaerial exposure and riverine input. Thus, the generated δ 34 S CAS data deliver not only valuable paleoecological and paleoenvironmental information, they also illustrate a heterogeneity in the seawater sulfate sulfur isotopic composition of the western Gondwanan ocean. Consequently, the lack of correlation between our Gondwanan δ 34 S CAS data and time equivalent sections of Laurentia and Siberia is probably not only caused by the absence of an internationally accepted biostratigraphic correlation, but rather supports the view that sulfate was non-conservative anion in seawater during the Cambrian Period.