This thesis explores mechanisms that determine coal seam gas (CSG) distribution and methods for its delineation. Understanding the distribution of gas content and composition underpins exploration and forecasting, as well as estimation of fugitive emissions from coal mines. Coal seam gas origins are variable, and thermogenic hydrocarbon accumulations are often supplemented by inorganic carbon dioxide and microbial methane in many reservoirs. The generation of these gases is dependent on geological and hydrogeological parameters relating to reservoir geometry and permeability.Specifically, this thesis examined: Hydro-geochemical controls on gas distributions and the apparent vertical zonation of gas reservoirs in the Sydney Basin, Australia; The role of in situ stress in regulating water and gas migration (and/or accumulation); and Utilisation of wireline temperature logging to enhance existing gas and geological exploration methods.The Sydney Basin is a coal-bearing sedimentary basin in eastern Australia. It is bounded by a series of highlands in the north, west and south and drains towards the centre and then to the east of the basin. Coal seam gas occurrence is laterally extensive and comprises layers of biogenic and thermogenic hydrocarbons and carbon dioxide. The zonation of these gases is regular and cross-cuts regional bedding dip; however, the sequence of gases varies with geographical position within the basin. Inland areas host a CO 2 -rich zone between the shallow biogenic and deep thermogenic hydrocarbon layers, whereas coastal locations are devoid of CO 2 , even in the vicinity of igneous intrusives.Gas contents typically increase with depth and peak at around 600-800m, below which volumes decrease to the base of the coal-bearing sequences. Carbon isotope data mirror this trend; both δ 13 C-CH 4 and δ 13 C-CO 2 increase with depth down to 800m, and then stabilise. These results confirm the respective biogenic and thermogenic hydrocarbon origins; however, carbon dioxide results are more complex. Conventional interpretation of CO 2 origin is limited to deep-seated magmatic sources; however, many of the δ 13 C-CO 2 ii values in the basin are outside of the traditionally assigned range. Investigations reveal that meteoric water enriched with positive cations (such as fresh rainwater in highland recharge areas) routinely dissolve carbonate mineralisation and transport bicarbonate down-gradient. Groundwater chemistry evolves along flow paths from fresh to saline composition and this causes re-precipitation of minerals. In some areas, the bicarbonate saturated waters can get trapped and, due to partial-pressure and groundwater salinity changes, liberate CO 2 gas which then adsorbs to the coal matrix. Saline groundwaters in coastal regions preclude the development of CO 2 -rich gas accumulations, instead hosting extensive hydrocarbon reservoirs.Groundwater infiltration and gas migration are dependent on permeability that primarily occurs via fractures and coal cleats. Horizontal stress is critica...