We have developed a new class of sodium carbonate/silicone composite sorbents that selectively capture carbon dioxide (CO2) and can purify biogas to natural gas pipeline-quality biomethane. These nontoxic composites can be three-dimensionally printed or extruded at low costs, can have high specific CO2 sorption rates (in excess of 5 μmol s-1 g-1 bar-1) and high selectivity due to their chemical mechanism, and can be regenerated with low-energy air stripping. Therefore, these composite sorbents combine the high selectivity of liquid sorbents with the high specific sorption rates and low regeneration energies found in many solid sorbents. We characterized these composite sorbents with X-ray computed tomography, scanning electron microscopy (SEM), and X-ray diffraction (XRD). Furthermore, we measured composite sorption capacities of up to 0.62 mol CO2 kg-1 and recorded breakthrough curves in a flow-through, fixed-bed reactor using both simulated biogas and locally sourced industrial biogas. Additional tests of the composite sorbent were carried out with pure CO2 in a sealed pressure drop apparatus. This experimental data was used to validate a numerical model of the setup and to simulate an industrial-scale biogas upgrading process. Finally, we performed a preliminary technoeconomic analysis for this upgrading process and found that this composite sorbent can upgrade biogas at a lower cost (∼$0.97 per GJ) than other currently implemented techniques.