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 (Vm/Vs). Vm/Vs 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 Vm/Vs 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 Vm/Vs value. With roughly the same micropore volume, pelletization alone increased Vm/Vs of coal carbon by 10%. Tire-derived carbons had Vm/Vs 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, Vm/Vs 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.