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Various compositional, depositional and maturity related influencing factors affect the complex pore structure of coal. To study the pore structural evolution at nanoscale, a well characterized sample set of vitrinite-rich Carboniferous coals from the Ukrainian Donets Basin, covering a maturity interval from 0.69 to 1.47%Rr, was selected. Conventional bright field transmission electron microscopy (BF TEM) and high-resolution TEM (HRTEM) imaging was used to directly determine pore size distributions, pore morphology, geometry factors and other structural features, while gas invasion techniques such as low-pressure gas adsorption (CO₂ and N₂) were used for the investigation of micro- and mesopore structural parameters. High-pressure CH₄ sorption experiments revealed changes in the methane storage capacity within the investigated maturity range, while associated structural changes of vitrinite were monitored …