The Upper Paleozoic (Carboniferous to Permian) succession in the east margin of the Ordos Basin in the North China Craton has a potential to contain significant hydrocarbon resources, though attention have been mainly attracted for its successful development of coalbed methane (CBM). To improve the previous resource estimates and evaluate the hydrocarbon play possibilities, this study incorporated new discoveries of hydrocarbon units and their stratigraphic relation with source rocks, hydrocarbon migration and trapping configurations. Continuous hydrocarbon accumulation units were identified within the Upper Paleozoic, including the Taiyuan, Shanxi and Xiashihezi formations with great tight gas potential, and the Taiyuan and Shanxi formations also containing shale gas and CBM. Different strata combinations are identified with coal deposition and favour for continuous gas accumulations, including the tidal flat, deltaic and fluvial systems distributed in most of the study areas. Methane was not only generated from the thick coal seams in the Taiyuan and Shanxi formations, but also from shale and dark mudstones. The coal, shale and tight sandstones are proved of remarkable gas content and hydrocarbon indications, and the gas saturation of tight sandstones decreases upward. The stacked deposit combinations vary isochronally in different areas, while the coal seams were developed stably showing good gas sources. Two key stages control the hydrocarbon enrichment, the continuous subsidence from coal forming to Late Triassic and the anomalous paleo-geothermal event happened in Early Cretaceous, as indicated by the fluid inclusions evidence. Extensive areas show good hydrocarbon development potential presently, and more works should be focused on the evaluation and selection of good reservoir combinations.