Abstract: There is great controversy regarding the origin and source of natural gas in the Lower Triassic Feixianguan Formation in the Eastern Sichuan Basin. This seriously restricts the study of natural gas dynamics in the Feixianguan Formation and thus hampers natural gas exploration in the region, so further study is urgently required. Using experimental tests of natural gas composition, stable isotopes, and noble gas isotopes with gas chromatography (GC) and mass spectrometry (MS) studies of source rock and reservoir asphalt saturated hydrocarbons, the natural gas geochemical characteristics, the genetic identification and a gas-source comparison of the Feixianguan Formation were studied. Then, constrained by the thermal history, the histories of gas generation and expulsion were restored by basin simulation technology. Finally, a gas accumulation model was established for the Feixianguan Formation. The results showed that (1) the H2S-rich and H2S-poor gas reservoirs of the Feixianguan Formation are distributed on the east and west sides of the Kaijiang-Liangping trough in the Eastern Sichuan Basin, respectively. The carbon and hydrogen isotope compositions of the natural gas in the gas reservoirs are generally heavy and have typical characteristics of high-maturity dry gas reservoirs. (2) The natural gas of the Feixianguan Formation is organic thermogenic gas, which is mainly oil-type gas generated by the secondary cracking of crude oil. The gas-generating parent material is mainly type II kerogen. (3) The natural gas of the Feixianguan Formation in the Eastern Sichuan Basin was mainly generated by argillaceous source rocks of the Upper Permian Longtan Formation. (4) Natural gas accumulation occurred as follows: the paleo-structure heights were filled with crude oil in the Early Jurassic, and paleo-oil reservoirs were formed in the Feixianguan Formation; during the Middle-Late Jurassic, the paleo-oil reservoirs were cracked when the reservoir temperatures rose above 160 °C, and paleo-gas reservoirs were formed. Since the end of the Late Jurassic, the paleo-gas reservoirs have been adjusted and reformed to form the present-day natural gas reservoirs. These results provide a basis for studying natural gas accumulation dynamics of the Feixianguan Formation in the Eastern Sichuan Basin.