A series of 2-benzoimidazol-8-ethoxyquinolines (L1–L6) and the nickel dihalides thereof (C1–C12) were synthesized and characterized by elemental analysis and infrared spectroscopy. The molecular structures of representative complexes were determined by single crystal X-ray diffraction which revealed a distorted pyramidal geometry at nickel. All complexes, when activated with Et2AlCl, showed high activities towards ethylene oligomerization and enhanced thermodynamic stability.