Here in we have grown bulk single crystals of NaAu2 for the first time to enable surface studies on the nature of the (111) bulk surface. This intermetallic compound exhibits surprisingly high catalytic activity for CO oxidation, a benchmark reaction. Theory predicts NaAu2 to be the most thermodynamically stable composition in the Na-Au binary phase diagram and NaAu2 has been seen to preferentially form in experiments containing Na and Au which supports this prediction. The (111) surface was also predicted to be the most stable and is nearly bulk-terminated making single crystal samples prepared with this crystallographic orientation a fitting choice. The crystal quality and surface composition of the metallographically prepared surface was determined by x-ray diffraction methods in addition to optical and electron microscopy.