Many -rich (up to 97% by volume) natural gas pools have been found in the continental margin basins of the northern South China Sea. By combining the geochemical data from 53 samples with their geologic backgrounds, this study investigated the origins and accumulation mechanism of , and discussed the role of in driving oil as it charged the reservoirs. The results reveal that the gases in the Yinggehai basin originate mainly from the thermal decomposition of both Miocene calcareous shales and Paleozoic carbonates, and that from mantle degassing is only a minor contributor. The accumulations in the Yinggehai basin are mainly controlled by diapiric faults and episodic thermal fluid movements. The gases in the eastern Qiongdongnan and western Pearl River Mouth basins are mainly related to magmatic or mantle degassing, and the volatiles from magmatic degassing during the igneous intrusion stage are the most likely major source of in these reservoirs, with basement faults providing pathways for upward migration of -rich mantle fluids. Natural displacements of oil by appear to be common in the eastern Qiongdongnan and western Pearl River Mouth basins. The -flooded oil or gas reservoirs have two common features that the present gas pools or oil-bearing structures have residual oils representing prior charge, and are close to the basement faults that provide pathways along which the mantle-derived -rich gas was migrated. The oils from prior hydrocarbon reservoirs have been naturally driven out by to form secondary oil reservoirs in the eastern Qiongdongnan and western Pearl River Mouth basins. Therefore, a full understanding of the origin and distribution of cannot just be used to trace hydrocarbon migration pathways, but also provide useful information for risk assessment prior to drilling.