The global Precambrian–Cambrian system includes an important series of hydrocarbon-bearing strata. However, because rocks of this age are typically deeply buried, few petroleum exploration breakthroughs have been made, and the presence of source rocks remains somewhat controversial. Recently, commercial condensate and gas were discovered from the deep (∼6900 m [∼22,600 ft]) Zhongshen 1C (ZS1C) exploratory well drilled in the Tazhong uplift of the Tarim Basin, China, leading to renewed interest in the development of Cambrian source rocks in the basin. On the basis of outcrop reconnaissance and sample testing from around the Tarim Basin, we show that a set of high-quality source rocks were developed within the lower Cambrian Yuertusi Formation (Є1y), at the base of the lower Cambrian. These rocks are black shales and typically have a total organic carbon content between 2% and 6% but extending as high as 17% in selected regions. This marine sequence is 10–15 m (33–49 ft) thick in some outcrops along the margins of the basin. Seismic data indicate that these high-quality source rocks may cover an area as large as 260,000 km2 (100,000 mi2). Their main organic parent material was benthic multicellular algae. On the basis of high-temperature thermal simulations conducted on these source rocks, we show that the gas composition and carbon isotopes from the ZS1C well are similar to the products generated at a thermal evolution stage corresponding to a vitrinite reflectance of between 2.2% and 2.5%. Late-stage natural gas accumulated within these rocks over time. The δ34S correlation of organic sulfur compounds in the condensate with Cambrian sulfates provides further evidence for a Є1y source rock origin of the ZS1C condensate and gas. The Cambrian dolomites in association with a salt seal exhibit favorable geological conditions for large-scale hydrocarbon accumulation. A new set of deep exploration strata can, therefore, be developed, guiding future deep Cambrian hydrocarbon exploration in the Tarim Basin.