Nickel-carbon composite materials (NiC catalysts) are synthesized by decomposing methane over Raney-type skeletal nickel catalysts. The NiC catalysts are evaluated in the hydrogenation of cyclooctene, cyclooctadiene, nitrobenzene, and para-chloronitrobenzene. Characterization by scanning electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy reveals that the catalysts consist of nickel in its metallic form with superficial oxide layers, carbon, and aluminum oxide/hydroxide. The catalysts exhibited excellent hydrogenation activity, superior to the parent Raney nickel.