In order to find out the enrichment mechanism and forming type of deep shale gas, taking the Longmaxi Formation shale in the Desheng–Yunjin Syncline area of Sichuan Basin as an example, we determined the mineralogy, organic geochemistry, physical property analysis, gas and water content, and the influence of three factors, namely sedimentation, structural conditions, and hydrogeological conditions, on the enrichment of shale gas. The results show that Longmaxi Formation shale in Desheng–Yunjin Syncline area is a good hydrocarbon source rock that is in the over-mature stage and has the characteristics of high porosity, low permeability, and high-water saturation. The contents of clay and quartz are high, and the brittleness index is quite different. According to the mineral composition, nine types of lithofacies can be found. The development characteristics of Longmaxi Formation shale and the sealing property of the roof have no obvious influence on the enrichment of shale gas, but the tectonic activities and hydrodynamic conditions have obvious influence on the enrichment of shale gas. The main control factors for shale gas enrichment in different regions are different. According to the main control factors, the gas accumulation in the study area can be divided into three types: fault-controlled gas, anticline-controlled gas, and hydrodynamic-controlled gas. The fault-controlled gas type is distributed in the north of the Desheng syncline and the north of the Yunjin syncline, the anticline-controlled gas type is distributed in the south of the Desheng syncline and the south of the Yunjin syncline, and the hydrodynamic-controlled gas type is distributed in the middle of the Baozang syncline. This result is of great significance for deep shale gas exploration.