Prompted by the ability of fullerene materials to promote formation and cleavage of strong bonds and participate in hydrogen-transfer reactions, we investigated fullerene-based materials for conversion of methane into higher hydrocarbons. Fullerene soot was found to activate the C-H bond of methane, allowing methane conversions at temperatures lower than those required under either purely thermal conditions or when other carbons such as Norit or acetylene black are used. Modification of the soot by extraction to remove the soluble fullerenes or by CO2 activation to produce a high surface area material did not significantly alter the catalytic activity. The use of an alkali metal such as potassium was found to dramatically increase the selectivity to C-2-C-4 hydrocarbons after an initial activation period at 950 degrees C.