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Australia is about to become the premier global exporter of liquefied natural gas (LNG), bringing increased opportunities for helium extraction. Processing of natural gas to LNG necessitates the exclusion and disposal of nonhydrocarbon components, principally carbon dioxide and nitrogen. Minor to trace hydrogen, helium and higher noble gases in the LNG feed-in gas become concentrated with nitrogen in the non-condensable LNG tail gas. Helium is commercially extracted worldwide from this LNG tail gas. Australia has one helium plant in Darwin where gas (containing 0.1% He) from the Bayu-Undan accumulation in the Bonaparte Basin is processed for LNG and the tail gas, enriched in helium (3%), is the feedstock for helium extraction. With current and proposed LNG facilities across Australia, it is timely to determine whether the development of other accumulations offers similar potential. Geoscience Australia has obtained helium contents in ~800 Australian natural gases covering all hydrocarbon-producing sedimentary basins. Additionally, the origin of helium has been investigated using the integration of helium, neon and argon isotopes, as well as the stable carbon (13C/12C) isotopes of carbon dioxide and hydrocarbon gases and isotopes (15N/14N) of nitrogen. With no apparent loss of helium and nitrogen throughout the LNG industrial process, together with the estimated remaining resources of gas accumulations, a helium volumetric seriatim results in the Greater Sunrise (Bonaparte Basin) > Ichthys (Browse Basin) > Goodwyn–North Rankin (Northern Carnarvon Basin) accumulations having considerably more untapped economic value in helium extraction than the commercial Bayu-Undan LNG development.