The Tarim Basin is located in northwestern China and is the biggest basin in China with huge oil and gas resources. Especially the Lower to Middle Cambrian and Middle to Upper Ordovician possess the major marine source rocks in the Tarim Basin and have large shale gas resource potential. The Cambrian–Ordovician shales were mainly deposited in basin–slope facies with thicknesses between 30–180 m. For shales buried shallower than 4500 m, there is high organic matter abundance with TOC (total organic carbon) mainly between 1.0% and 6.0%, favorable organic matter of Type I and Type II, and high thermal maturity with RoE as 1.3%–2.75%. The mineral composition of these Cambrian–Ordovician shale samples is mainly quartz and carbonate minerals while the clay minerals content is mostly lower than 30%, because these samples include siliceous and calcareous shale and marlstone. The Cambrian and Ordovician shales are compacted with mean porosity of 4% and 3%, permeability of 0.0003×10?3–0.09×10?3 μm2 and 0.0002×10?3–0.11×10?3 μm2, and density of 2.30 g/m3 and 2.55 g/m3, respectively. The pores in the shale samples show good connectivity and are mainly mesopore in size. Different genetic types of pores can be observed such as intercrystal, intergranular, dissolved, organic matter and shrinkage joint. The reservoir bed properties are controlled by mineral composition and diagenesis. The maximum adsorption amount to methane of these shales is 1.15–7.36 cm3/g, with main affecting factors being organic matter abundance, porosity and thermal maturity. The accumulation characteristics of natural gas within these shales are jointly controlled by sedimentation, diagenesis, hydrocarbon generation conditions?, reservoir bed properties and the occurrence process of natural gas. The natural gas underwent short-distance migration and accumulation, in-place accumulation in the early stage, and adjustment and modification in the later stage. Finally, the Yulin (well Y1) and Tazhong (well T1) areas are identified as the targets for shale gas exploration in the Tarim Basin.