The Archean Tati greenstone belt is located at the southwestern margin of the Zimbabwe craton (northeast Botswana) and hosts numerous Cu-Ni ± platinum group element (PGE) and Au ± Ag occurrences and deposits. Gold occurrences/deposits are poorly studied, and key questions pertaining to their genesis remain unclear, including the mode of occurrence(s) of gold, the relative timing of gold introduction with respect to the evolution of the greenstone belt, the number of gold mineralization events, the alteration patterns, and the relationships between each alteration pattern and gold mineralization. A detailed study that includes sulfide and gold grain chemistry using laser ablation-inductively coupled plasma-mass spectrometry (LA-ICP-MS) and electron probe microanalysis (EPMA), respectively, and X-ray diffraction (XRD) of mineralized rock samples of three Tati greenstone belt gold deposits was carried out to constrain the genesis of gold mineralization and formulate exploration guidelines in the Tati greenstone belt. Gold in the Tati greenstone belt is the result of multiple events, is mainly associated with arsenopyrite, pyrite, and sphalerite, and occurs as (1) microinclusions within sulfides, (2) intergrowth with sulfides, (3) minute particles (<2–10 μm) within the silicate matrix, (4) microfractures and microvug infills, and (5) lattice-bound and sulfide-hosted refractory gold. The first gold event (as electrum) is premetamorphic and associated with sphalerite-quartz veins. The second stage is a postmetamorphic high-grade gold event that is accompanied by extensive carbonatization and propylitization of host rocks. The third stage of gold mineralization is marked by the dissolution of gold in the early formed stages 1 to 2 and subsequent reprecipitation within cracks, fractures, and vugs. Auriferous pyrite composition suggests that Au-bearing mineralizing fluids are predominantly of magmatic origin and that their physicochemical compositions changed during the mineralization process, as supported by chemically zoned Au-bearing arsenopyrite, various alteration types containing gold, and variation in gold fineness across the several gold deposits in the Tati greenstone belt. Gold deposition in the Tati greenstone belt mainly occurred through sulfidation, as indicated by the closest spatial association between gold and Fe-bearing sulfides and ferromagnesian silicates. Gold in the Tati greenstone belt is closely correlated with As, Sb, Pb, Bi, Ni, Hg, Tl, Cd, In, Mo, W, Zn, and Te and moderately to weakly associated with Sn, Se, Cr, Co, Ge, Cd, Mn, V, Ga, and Ag. The correlation between Au and fluid mobile elements, i.e., Te, Sb, Se, As, Hg, and Bi, can be used as a vectoring tool during the exploration of gold within the Tati greenstone belt, as these elements likely form halos that are much broader than the primary footprint of gold mineralization.