The azaferrocenyliminonickel dibromide complexes 1 bearing a pentaphenylcyclopentadienyl group and a wide range of N-aryl groups were synthesized and examined as catalysts for ethylene polymerization. Both the ortho-(R-1) and para-substituents (R-2) of the N-aryl groups in 1 were found to strongly influence both the polmerization activity and the properties of the obtained polyethylenes. The effect of changing the polymerization conditions, such as temperature, ethylene pressure, and cocatalyst, was also examined.