Petrographic and sulphur isotope studies support the long-held contention that rounded grains of pyrite in siliciclastic sequences of the Late Archaean Witwatersrand Supergroup originated as placer grains. The grains are concentrated at sites where detrital heavy minerals are abundant within quartz-pebble conglomerates and quartzose sandstones. Depositional sites with abundant pyrite are: (1) within the matrix of bar-type, clast-supported conglomerates; (2) on scoured or winnowed surfaces; and (3) on stratification planes. The grains are internally compact or porous, with truncation of internal structure at outer margins indicating fragmentation and rounding of pyritic source-rocks during erosion and sediment transport. A large range in textures reflects source-rock lithologies, with known varieties linked to sedimentary-hosted diagenetic pyrite, volcanic-hosted massive sulphide deposits and hydrothermal pyrite. Laser ablation sulphur isotope analysis of pyrite reveals a broader range in delta(34)S values (-5.3 to +6.7parts per thousand) than that of previously reported conventional bulk-grain analyses (1 to +4parts per thousand). Rounded pyrite from the Steyn Reef has significant variation in delta(34)S values (-4.7 to +6.7parts per thousand) that establishes heterogeneous sulphur compositions, with even adjacent grains having diverse isotopic signatures. The heterogeneity supports a placer origin for rounded pyrite. Euhedral pyrite and pyrite overgrowths which are undoubtedly authigenic have restricted delta(34)S values (-0.5 to + 2.5parts per thousand), are chemically distinct from rounded pyrite and are probably the products of metamorphism or hydrothermal alteration. The placer origin of rounded pyrite indicates that pyrite was a stable heavy mineral during erosion and transport in the early atmosphere. Its distribution in three sequences (Witwatersrand Supergroup, Ventersdorp Contact Reef and Black Reef), and in other sequences not linked to Witwatersrand-type Au-U ore deposits, implies deposition of redox-sensitive detrital heavy minerals during the Late Archaean. Consequently, rounded grains of detrital pyrite are strong indicators of an oxygen-poor atmosphere. While not confirming a placer origin for gold in Witwatersrand Au-U ore deposits, the palaeoenvironmental significance of rounded pyrite negates its link to hydrothermal mineralization.