The lacustrine shales in the Lodève Basin, southern France, serve as excellent archives of paleo-lake development as well as climatic evolution during the Early Permian. In this study, an extensive dataset is presented encompassing organic petrographic data, major and trace element quantification, bulk and molecular organic geochemical proxies, as well as compound-specific stable carbon isotope data derived from the analysis of 36 black shale outcrop samples originating from the Usclas-St. Privat Formation (USPF), Tuilières-Loiras Formation (TLF), and Viala Formation (VF). All sample are thermally oil-mature, as evident from a vitrinite reflectance (VRr) of around 0.8%. The lower section of the USPF, characterized by notably higher total sulfur (TS) concentrations, displays total organic carbon (TOC) and TS contents spanning from 2.69 to 7.83 (avg. 4.28) wt% and 0.42–1.55 (avg. 1.09) wt%, respectively. In contrast, the upper section of the USPF (average TOC of 2.59 wt%), TLF (average TOC of 2.66 wt%), and VF (average TOC of 3.17 wt%) exhibit considerably lower TS contents of 0.26 wt%, 0.22 wt%, and 0.17 wt%, respectively. The lower section of the USPF, characterized by the lowest pristane/phytane (Pr/Ph) ratio and the highest TS/TOC ratios and chemical index of alteration (CIA) values, was deposited in oxygen-depleted and saline lacustrine environments. These conditions prevailed under more humid climatic conditions and were probably related to marine incursions. In contrast, the upper section of the USPF, the TLF, and the VF display elevated Pr/Ph ratios but reduced TS/TOC and CIA values, signifying deposition within oxic-dysoxic and freshwater-brackish bottom water conditions with a significant change towards arid conditions. All samples are characterized by low vitrinite and inertinite contents together with consistently similar average values of Al2O3 and TiO2. The biomarker analysis suggests that the organic matter (OM) in most samples mainly originates from planktonic/algal biomass with additional microbial OM. Only the lower section of the USPF displays a slightly enhanced contribution of terrestrial OM input and also more detrital elements. It is concluded that the structural evolution of the basin from narrow deep towards wider and shallower settings as well as the postulated marine transgressive events during early stages played a crucial role in shaping the deposition environments of the two distinct sets of lacustrine shales, thereby influencing the OM accumulation mechanisms. In contrast, the substantial climatic aridification seems to have a relatively minor impact on the sources of OM and the conditions prevailing within the water column.