Accurate testing coal isotherm can play a significant role in the areas of coal seam gas drainage, outburst control, CO2 geo-sequestration, coalbed methane (CBM) and enhanced coalbed methane recovery (ECBM) etc. The effect of particle size on the CO2 and CH4 sorption capacity of bituminous coal from Illawarra, Australia was investigated at 35°C and at pressure up to 4 MPa. A unique indirect gravimetric apparatus was used to measure the gas adsorption and desorption isotherms of coal of different particle sizes ranging from around 150 urn to 16 mm. Langmuir model was used to analysis the experimental results of all gases. Coal particle size was found to have an apparent effect on the coal ash content and helium density results. Coal with larger particle size had higher ash content and higher helium density. The sorption isotherm was found to be highly sensitive with helium density of coal which was determined in the procedure of testing the void volume of sample cell. Hence, coal particle size had a significant influence on the coal sorption characteristics including sorption capacity and desorption hysteresis for CO2 and CH4, especially calculated with dry basis of coal. In this study, the 150-212 um (150 um) coal samples achieved higher sorption capacity and followed by 2.36-3.35 mm (2.4 mm), 8-9.5 mm (8 mm) and 16-19 mm (16 mm) particle size samples. However, the differences between different coal particles were getting smaller when the sorption isotherms are calculated with dry ash free basis. Test with 150 um coal samples were also found to have relatively smaller desorption hysteresis compared with the other larger particle size samples. The different results including adsorption/desorption isotherm, Langmuir parameters and coal hysteresis were all analysed with the CO2 and CH4 gases.