Natural gases from all of Australia’s major gas provinces in the Adavale, Amadeus, Bass, Bonaparte, Bowen/ Surat, Browse, Canning, Carnarvon, Cooper/Eromanga, Duntroon, Gippsland, Otway and Perth basins have been examined using molecular and carbon isotopic compositions in order to define their source, maturity and secondary alteration processes.The molecular compositions of the gaseous hydrocarbons range from highly wet to extremely dry. On average, reservoired gases predominantly derived from land plants are slightly wetter than those derived from marine sources. The non-hydrocarbon gases CO2 and N2 were sourced from both inorganic and organic materials. A mantle and/or igneous origin is likely in the majority of gases with CO2 contents >5%. For gases with lower CO2 contents, an additional organic input, associated with hydrocarbon generation, is recognised where δ13C CO2 is A strong inter-dependency between source and maturity has been recognised from the carbon isotopic composition of individual gaseous hydrocarbons. This relationship has highlighted some shortcomings of common graphical tools for interpretation of carbon isotopic data. The combination of the carbon isotopic composition of gaseous hydrocarbons and the low molecular weight nalkanes in the accompanying oil allows our knowledge of oil-source correlations and oil families to be used to correlate gases with their sources. This approach has identified source rocks for gas ranging in age from the Ordovician in the Amadeus Basin to Late Cretaceous- Early Tertiary sources in the Bass and Gippsland basins. The carbon isotopic composition of organic matter, approximated using the δ13C of iso-butane, shows a progressive enrichment in 13C with decreasing source age, together with marine source rocks for gas being isotopically lighter than those from land plant sources. The Permian was a time when organic matter was enriched in 13C and isotopically uniform on a regional scale.Secondary, in-reservoir alteration has played a major role in the modification of Australian gas accumulations. Thus, biodegradation, prominent in the Bowen/Surat, Browse, Carnarvon and Gippsland basins, is found in both hydrocarbon and non-hydrocarbon gases. This is recognised by an increase in gas dryness, elevated isoalkane to n-alkane ratio, differential increase in δ13C of the individual wet gas components, a decrease in δ13C of methane and a reduction in CO2 content concomitant with enrichment in 13C. Evidence of water-washing has been identified in accumulations in the Bonaparte and Cooper/Eromanga basins, resulting in an increase in the wet gas content. Seal integrity is also a major risk for the preservation of natural gas accumulations, although its effect on gas composition is only evident in extreme cases, such as the Amadeus Basin, where preferential leakage of methane in the Palm Valley field has resulted in the residual methane becoming enriched in 13C.The greater mobility of gas within subsurface rocks can have a detrimental effect on oil composition whereby gas-stripping of light hydrocarbons is common amongst Australian oil accumulations. Alternatively, the availability of gas, derived from a source rock common to or different from oil, was likely to have been a prime factor controlling the regional distribution of oil, whereby mixing of both results in increased oil mobility and can lead to a greater access to the number and types of traps in the subsurface.