Methane (CH3D) is formed directly by abstraction by methyl radicals of adsorbed D on a Ni(lll) surface. This reaction occurs at a surface temperature of 120 K and in the presence of open metal binding sites. A direct reaction by unaccommodated methyl radicals is involved, since accommodated methyl radicals on Ni(lll) react only above 200 K. Modeling efforts show that the cross section for accommodation of methyl radicals to open metal sites is approximately five times larger than that for D abstraction.