Dual-reflux pressure swing adsorption (DR PSA) processes using a kinetically nitrogen selective molecular sieve carbon, MSC-3K 172, were investigated for the removal of nitrogen from a gas mixture consisting of 75 mol% CH4 + 25 mol% N-2. The four DR PSA configurations (PL-A, PH-A, PL-B and PH-B) were experimentally demonstrated and compared in terms of their nitrogen rejection and methane recovery performance. The experimental results indicated the PH-B configuration in general performed the best in terms of the methane product purity and recovery using the kinetic MSC-3K 172 adsorbent. A non-isothermal numerical model was constructed for the kinetic DR PSA process to simulate and optimise the performance of the PH-B configuration. Model predicted gas loadings on the adsorbent indicated that selectively removing nitrogen from methane was feasible when a feed step time close to the characteristic adsorption time of nitrogen was selected. The effective usage of the adsorption bed in the PH-B configuration was also numerically studied via the capacity ratio C, with the feed step time and light reflux flow as key operational parameters, at fixed heavy product-to-feed ratio, bed pressure ratio and feed location. The numerical model for the PH-B configuration was also employed to study the effect of pressure in the purge step beyond those conditions accessible in the experiment. The simulation results revealed that the PH-B configuration could achieve a separation performance of 90 mol% CH4 in the light product with 90% CH4 recovery when the pressure in the light purge column was lower than 40 kPa while the adsorption pressure was maintained at 500 kPa. This result opens new opportunities for efficiently upgrading sub-quality natural gas reserves.