The paper presents research on the influence of grain size of selected coals and their structural parameters on the diffusion coefficient and methane sorption isotherms. Two coals from Polish hard coal mines, differing in the coal rank, were tested. Sorption isotherms for methane were determined. An unconventional sequence of pressures 0→0.1→0→0.5→0→1.5 MPa was employed to assess the speed of achieving sorption equilibrium at different pressures. The studies of CH4 accumulation kinetics were performed on various grain classes of the tested coals. Both the sorption capacity of coal and the diffusion coefficient proved to be highly sensitive to the experimental methodology. Critical measurement parameters in terms of determining the diffusion coefficient concerning the assumptions of the Crank model were indicated. The influence of the equivalent radius of coal grain on the process kinetics was demonstrated. The stepwise pressure increase factor was examined in the context of minimising the impact of sorption isotherm non-linearity on the results. The importance of the width of the grain class of coals was determined to reduce their maceral inhomogeneities. These factors are the most common reason that makes it difficult to quantitatively compare diffusion coefficient values.