The partial oxidation of methane towards synthesis gas is catalyzed over calcium aluminate (CaO-2Al(2)O(3)) catalysts, either unpromoted or promoted with small amounts of Ni (0.1-0.5 wt%), at medium temperatures (800 degrees C) and methane-to-oxygen ratios of 2:1. Carbon monoxide and hydrogen appear to be primary products of the reaction, along with carbon dioxide and small amounts of C-2+ hydrocarbons. Methane conversions of 35% and carbon monoxide-to-carbon dioxide ratios of 0.5-0.6 are obtained with the unpromoted or 0.1 wt% Ni-promoted catalysts at complete oxygen consumption. Near thermodynamic equilibrium synthesis gas mixtures are realized with the 0.5 wt% Ni-promoted calcium aluminate catalyst at sufficiently long gas contact times.