Abstract: Few studies have systematically investigated the factors controlling organic matter enrichment in shales from the Qiongzhusi Formation, within and surrounding the Sichuan Basin, under different depositional environments. This has resulted in different academic understandings and limited clarity on the mechanisms of organic matter enrichment. On this premise, in this study, the basic geological characteristics and depositional paleoenvironments of shales along the passive continental margin, the western Hubei Trough, and the western Sichuan Trough were compared and analyzed using core, outcrop, and mineral testing. Furthermore, data from organic geochemical and elemental analyses were utilized to investigate the different enrichment mechanisms and formation modes of the organic matter in different periods. The results reveal that the organic matter enrichment in this region should be mainly influenced by the preservation conditions, paleo-productivity, and terrigenous input. However, there were clear differences in the main controlling factors in the different periods. In the Q1 phase, the region had a high sea level, had the strongest rifting, had the largest accommodation space, and exhibited characteristics of low terrestrial input and bottom water hypoxia. The changes in the paleo-productivity caused by upwelling currents were the main factors controlling the variations in the organic matter enrichment. In the Q2 phase, the weakened decreasing sea level co-occurred with a reduction in the accommodation space across the region. The organic matter enrichment was significantly controlled by the paleo-productivity, preservation conditions, and terrigenous inputs, and the organic matter enrichment conditions deteriorated from the passive continental margin to the western Hubei Trough and western Sichuan Trough. The total organic carbon (TOC) content of the shale decreased significantly. In the Q3 phase, the entire region entered an infilling stage, which was dominated by an oxygen-rich environment, and the preservation conditions were the decisive factor controlling the organic matter enrichment. The TOC content was low overall, and there were no evident differences across the different zones.