In this study, molecular sieving carbons (MSCs) for biogas upgrading were successfully fabricated by a simple temperature controlled carbonization of moso bamboo (Phyllostachys pubescens) without energy consuming steps (i.e. char activation and pore modification). As the carbonization temperature increased from 600 to 900 °C, the specific surface area of bamboo charcoals increased and the pore size distribution of bamboo charcoal became narrower and closer to the dimensions of CH 4 (0.38 nm). Bamboo charcoals had a more disordered carbon stacking structure than commercial MSC and contained more surface oxides, which contribute to greater surface reactivity than commercial activated carbon. Bamboo charcoal carbonized at 900 °C had the highest CO 2 adsorption capacity (121.6 g kg −1), even higher than commercial MSC (102.88 g kg −1). Despite the poor kinetic CO 2 adsorption properties of bamboo charcoals compared to commercial MSC, synthetic biogas (60% CH 4 + 40% CO 2) was successfully upgaded to concentrated CH 4 (>90%) by small-scale pressure swing adsorption using bamboo charcoal. It is expected that bamboo charcoals can contribute to sustainable small-scale biogas upgrading.