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The major platinum group element (PGE) occurrence in the Great Dyke of Zimbabwe, the main sulfide zone, is a tabular stratabound layer hosted in pyroxenites, and it is broadly similar in form throughout the length of the Great Dyke. We conducted a petrographic and sulfide composition study on a sulfide-enriched zone from the contact of the mafic sequence–ultramafic sequence through the main sulfide zone at Unki Mine in the Shurugwi Subchamber to its underlying footwall rocks to place some constraints on the origin of the rocks.Pyrrhotite, pentlandite, chalcopyrite, and pyrite are the base metal sulfides that were encountered during the study. Pyrrhotite, pentlandite, and chalcopyrite typically occurred as inclusions in both primary (orthopyroxene, plagioclase, and clinopyroxene) and secondary (amphibole and chlorite) silicate phases, whereas pyrite was observed in only three samples, where it occurred in association with pyrrhotite. The concentrations of PGEs in the base metal sulfides were nearly all at or below minimum detection limits. The intercumulus nature of some of these sulfides in the investigated sequence suggests that they were likely formed during the crystallization history of these rocks. The occurrence of pyrite, which we interpret to be an alteration phase, suggests that a late-stage event, likely formed during hydrothermal alteration, helped to concentrate the mineralization at Unki Mine. In some cases, however, these sulfides occur partially surrounding some chromite and silicate phases. Thus, some sulfides in the Unki Mine area were likely formed early in the crystallization history of the Great Dyke, whereas others were formed late during hydrothermal processes. Low concentrations of PGEs such as platinum (Pt), palladium (Pd), and rhodium (Rh) in base metal sulfides imply that the PGEs in the main sulfide zone and Unki Mine are hosted either in silicates and/or platinum group minerals. Very low Co contents in pentlandites in the rocks under investigation are interpreted to imply that very limited Fe substitution by Co, and also of Ni by Co, occurred. Broadly comparable trends, with minor variations of Fe in pyrrhotite, of Co and Ni in pentlandite, and of Cu in chalcopyrite, for example, likely reflect magmatic processes. The concentrations of these metals in base metal sulfides vary sympathetically, indicating that their original magmatic signatures were subsequently affected by hydrothermal fluids. The spiked pattern displayed by the variations in the percent modal proportions of the base metal sulfides across the entire investigated stratigraphic section is interpreted to reflect remobilization of the sulfides during hydrothermal alteration. Depletions in some elements, which occur near the base and at the top of the investigated succession, are likely a result of this hydrothermal alteration.