A series of iron(II) dichloride complexes (Fe1–Fe7) ligated by 2-(2-benzoxazolyl)-6-[1-(arylimino)ethyl]pyridines was synthesized and characterized [aryl = 2,6-R12C6H3; R1 = Me (1), Et (2), iPr (3), Cl (4), Br (5); 2,6-Me2C6H2-4-R2, R2 = Me (6), Br (7)]. The molecular structures of Fe1, Fe3, and Fe5 were determined by the single-crystal X-ray diffraction. Complexes Fe1 and Fe3 both display distorted trigonal-bipyramidal geometries, whereas complex Fe5 is a distorted square pyramid. Upon activation with modified methylaluminoxane, all iron complexes showed moderate to good activities [up to ca. 106 g(product)?×?(mol Fe)–1 h–1?bar–1] for the oligomerization and polymerization of ethylene, with high selectivity for vinyl-terminated oligomers or polyethylene waxes.