The genesis of quartz vein-hosted gold mineralization in the Neoproterozoic–early Palaeozoic Dalradian Supergroup of Scotland remains controversial. An extensive new dataset of S-isotope analyses from the Tyndrum area, together with correlation of the global Neoproterozoic sedimentary S-isotope dataset to the Dalradian stratigraphy, demonstrates a mixed sedimentary and magmatic sulphur source for the mineralization. δ³⁴S values for early molybdenite- and later gold-bearing mineralization range from −2 to +12‰, but show distinct populations related to mineralization type. Modelling of the relative input of magmatic and sedimentary sulphur into gold-bearing quartz veins with δ³⁴S values of +12‰ indicates a maximum of 68% magmatic sulphur, and that S-rich, SEDEX-bearing, Easdale Subgroup metasedimentary rocks lying stratigraphically above the host rocks represent the only viable source of sedimentary sulphur in the Dalradian Supergroup. Consequently, the immediate host rocks were not a major source of sulphur to the mineralization, consistent with their low bulk sulphur and lack of metal enrichment. Recent structural models of the Tyndrum area suggest that Easdale Subgroup metasedimentary rocks, enriched in ³⁴S, sulphur and metals, are repeated at depth owing to folding, and it is suggested that these are the most likely source of sedimentary sulphur, and possibly metals, for the ore fluids.