The Paleoproterozoic Tanami Group of the Granites—Tanami Orogen hosts a known endowment of > 20 Moz of gold mineralization across numerous deposits. Throughout the region, host lithologies impart a first-order control on the style, grade and endowment of mineralization. However, the genetic relationship and regional distribution of three regionally correlative formations (the Dead Bullock, Mount Charles and Stubbins formations) remains enigmatic. Here, we combine lithostratigraphic analysis, lithogeochemistry, detrital zircon geochronology and geophysical observations to propose a new evolutionary model for the Tanami Group. We find that the Tanami Group was deposited in a continental back-arc basin setting and developed in four stages. Package A marked the onset of the rifting of the continental Archean basement. Sedimentary rocks within Package A are dominantly felsic in composition and display a unimodal detrital zircon age population at ∼ 2530 Ma. Package B marks the onset of mafic volcanism; consequently, volcaniclastic and sedimentary rocks within Package B display a distinct mafic geochemical signature. Detritus shed from an Archean basement persisted throughout this period, and a unimodal detrital age component at ∼ 2530 Ma persists. Package C marked the waning stages of voluminous mafic volcanism across the Tanami Basin. Sedimentary volcaniclastic rocks within Package C display a mixed mafic and felsic composition. Detrital zircon age spectra record multiple peaks at ∼ 2500, 3000 and 3350 Ma, which may reflect erosion of older Archean basement domains or changes in paleo-drainage. Package D marked a significant change in the source of detritus entering the basin from dominantly Archean to Paleoproterozoic, with dominant detrital age peaks at ∼ 1860 Ma. Despite significant lithofacies variations, the presented model highlights multiple correlations between the Dead Bullock and Mount Charles formations. The Mount Charles Formation likely represents a volcanic source-proximal, high-energy depocenter. In contrast, the Dead Bullock Formation was deposited in a lower energy setting, distal to volcanic centers. These observations are important to mineral exploration. Notably, the Mount Charles Formation is distributed over a significantly greater area than previously thought, and the under-represented Hangingwall and Footwall sequences of this formation are interpreted to host significant gold mineralization at the Oberon and Groundrush deposits.