Ph.D. ; Petrographic, chemical and multiple sulfur isotope analyses were conducted on pyrite from argillaceous, arenaceous and rudaceous sedimentary rocks from the Mesoarchean Witwatersrand Supergroup. Following detailed petrographic analyses, four paragenetic associations of pyrite were identified. These include: 1) Detrital pyrite (derived from an existing rock via weathering and/or erosion). 2) Syngenetic pyrite (formed at the same time as the surrounding sediment). 3) Diagenetic pyrite (formed in the sediment before lithification and metamorphism). 4) Epigenetic pyrite (formed during metamorphism and hydrothermal alteration). It was found that the distribution of the pyrite varies with respect to the stratigraphic profile of the Witwatersrand Supergroup and depositional facies within the Witwatersrand depository. In this regard, the four paragenetic associations of pyrite are either scarce or absent in marine-dominated depositional environments, which occur in the lower parts of the succession and in geographically distal parts of the depository. Conversely, the four paragenetic associations are well represented in fluvial-dominated depositional environments, which occur in the middle and upper parts of the succession and in geographically proximal parts of the depository. However, it is worth noting that diagenetic pyrite in the West Rand Group occurs as in situ segregations in carbonaceous shale, whereas syngenetic and diagenetic pyrite in the Central Rand Group occurs as reworked and rounded fragments in fluvial quartz-pebble conglomerates. The strong association between fluvial depositional environments and sedimentary pyrite (syngenetic and diagenetic pyrite) infers a continental source of the sulfur (sulfide weathering or volcanic activity), whereas the lack of pyrite in marine depositional environments is consistent with the model of a sulfate-poor Archean ocean. The connection between epigenetic pyrite and the fluvial-dominated depofacies is probably related to the elevated concentrations of precursor sulfides (i.e., remobilization of syngenetic and early diagenetic pyrite) and the presence of organic carbon (conversion of metal-rich early diagenetic pyrite into pyrrhotite and base metal sulfides). In support of the petrographic observations above, it was found that the trace element chemistry of each paragenetic association of pyrite yields a distinctive set of chemical compositions and interelement variations (Co, Ni and As contents). Regarding detrital pyrite, two chemical populations can be distinguished according to grain size: 1) small grains (tens of μm’s) with high levels of metal substitution (up to wt. %) and interelement covariation and iv 2) large grains (>100 μm) with low levels of metal substitution (≤200 ppm). These two populations are thought to represent pyrite derived from sedimentary and metamorphosed source areas, respectively (see below). The trace element chemistry of diagenetic pyrite varies relative to the Fe-content of the host rock. Diagenetic pyrite from Fe-rich host rocks, such as magnetic mudstone and banded iron formation (BIF), generally contain low Ni contents (