The late Paleozoic Fengcheng Formation shale (LPF shale) in the Junggar Basin, NW China, is the oldest alkaline source rock discovered in the world, providing a unique perspective with which to explore organic matter (OM) enrichment in alkaline lake environments. Combined with the organic carbon isotope profile and paleoenvironmental proxies, this study reveals that the LPF shale was deposited in an arid climate with high salinity and a strong reducing environment, accompanied by frequent volcanic activity. High TOC values are concentrated in two intervals with frequent fluctuations in OM types. A negative excursion due to changes in sedimentary OM source is found in the δ13Corg profile. The excursion corresponds to the OM enrichment interval and is accompanied by abnormally high values of Sr/Ba and Sr/Cu. This implies that the extreme arid climate has led to high salinity, resulting in strong reducibility and changes in paleontological assemblages, which in turn controlled the differential enrichment of OM. The Fengcheng Fm. high-quality source rocks are the result of the combined action of climatic events, volcanism, high-salinity water environment and superior hydrocarbon-generating organisms. The results provide new insights into the formation conditions of terrestrial alkaline high-quality source rocks and the factors controlling alkaline OM enrichment.