The effect of the oxidation degree of a nickel foil surface on the rate of catalytic oxidation of ethylene was studied by a pulse method at 600 and 700°C. It was shown that a reduced metallic surface demonstrated a high activity in partial ethylene oxidation, whereas a partially oxidized surface with an oxidation degree of ~24 formal O2 monolayers, in the total oxidation of C2H4. A SEM investigation has revealed that the oxidized surface was partially coated with nickel oxide nanocrystals. A further increase in the surface oxidation degree led to a continuous coverage of the Ni surface with oxide crystals and a dramatic decrease of catalytic activity. In addition, a low maximum of total ethylene oxidation was observed at 700°C in the range of surface oxidation degree of 95–135 O2 monolayers.