Knowledge of adsorption equilibrium and kinetic data is essential for the design of an adsorption process. In this work, the adsorption equilibrium isotherms of methane and nitrogen are reported at 303, 323, and 343 K over the pressure range from 0 to 700 kPa by a gravimetric system on a carbon molecular sieve (CMS-131510). Methane is preferentially adsorbed. The adsorption capacity at 303 K and 700 kPa is 1.91 mol/kg for methane and 1.01 mol/kg for nitrogen. Experimental data obtained were fitted with the multisite Langmuir model and Toth model. The adsorption kinetics of pure gas was studied by a batch uptake experiment at several different surface coverages within the pressure range of 0100 kPa and in the same temperature range covered by the equilibrium isotherm. The adsorption rate of both gases is found to be controlled by the surface barrier resistance at the mouth of the micropore and diffusion in the micropore interior. The dual resistance model employed in the simulation can successfully describe the uptake curves. The temperature and concentration dependences of kinetic parameters were also studied. A very high kinetic selectivity was observed. The effect of micropore distribution on the transport parameters is discussed in detail. Binary breakthrough curves were determined, and an enrichment of 50% for methane in the first few seconds was observed. The data reported in this work can be used for the future modeling of adsorption process for the separation of methane and nitrogen on this CMS material.