Spectral gamma ray log (SGRL) data has been widely employed to derive subsurface lithological information and to perform well correlation when the core is not available. Previous studies mainly targeted homogenous facies whereas few attempts addressed heterolithic successions. The SGRL investigation here aimed at deriving lithofacies and further constrain conditions of deposition prevailing during the early Jurassic (Mbuo, Nondwa, and Mihambia Fms.) in the Mandawa Basin, onshore Tanzania, where core and outcrop data is rare. By use of binary discrimination diagrams of U, Th, and K, composition fields were defined for various lithofacies types (black shale, red shale, siltstone, sandstone, chert, anhydrite, halite, and carbonate) compiled from literature data. Sediment composition for two wells in the Mandawa Basin was then deduced from cuttings and SGRL data and compared with literature-derived geochemical provenance data from adjacent regions and strata. Binary discrimination diagrams revealed the presence of multi-mineral components in the heterolithic facies type, which in concert with diagenetic and detrital mineral dilution effects, led to low compositional contrasts between provenance fields and to overlap of different lithofacies types, complicating interpretation and limiting the effectiveness of the SGRL-based facies differentiation. For the early Jurassic strata, an upward increase in the Th/K ratio suggests an enhanced terrigenous influx into the basin due to intensified weathering. High Th/U and Th/K in the study region indicate a relatively shallow, well mixed, and oxic depositional setting in proximity to the source area opposing the more distal, deeper, and reduced depositional settings that prevailed in the southern central part of the basin. Th/U and Th/K excursions in the Nondwa and Mihambia formations suggest a shift towards less oxic depositional conditions upon two major marine incursions, corroborated by a decline in the clastic fraction and concomitant increase in carbonate.