Activated carbons for natural gas storage were produced from Illinois bituminous coals (IBC-102 and IBC-106) and scrap tires by physical activation with steam or CO₂ and by chemical activation with KOH, H₃PO₄, or ZnCl₂. The products were characterized for N₂-BET area, micropore volume, bulk density, pore size distribution, and volumetric methane storage capacity (V_m/V_s). V_m/V_s values for Illinois coal-derived carbons ranged from 54 to 83 cm³/cm³, which are 35−55% of a target value of 150 cm³/cm³. Both granular and pelletized carbons made with preoxidized Illinois coal gave higher micropore volumes and larger V_m/V_s values than those made without preoxidation. This confirmed that preoxidation is a desirable step in the production of carbons from caking materials. Pelletization of preoxidized IBC-106 coal, followed by steam activation, resulted in the highest V_m/V_s value. With roughly the same micropore volume, pelletization alone increased V_m/V_s of coal carbon by 10%. Tire-derived carbons had V_m/V_s values ranging from 44 to 53 cm³/cm³, lower than those of coal carbons due to their lower bulk densities. Pelletization of the tire carbons increased bulk density up to 160%. However, this increase was offset by a decrease in micropore volume of the pelletized materials, presumably due to the pellet binder. As a result, V_m/V_s values were about the same for granular and pelletized tire carbons. Compared with coal carbons, tire carbons had a higher percentage of mesopores and macropores.