A series of half-titanocene dichloride 2-aryliminoquinolin-8-olates, CpTi LCl2 (C1–C6: Cp as C5H5, L as 2-(1-(o-benzhydrylarylimino)methyl)quinolin-8-olates or 2-(1-(o-benzhydrylarylimino)ethyl)quinolin-8-olates), was synthesized and fully characterized; the molecular structures of representative complexes C2 and C4 are reported. Upon activation with modified methylaluminoxane (MMAO), the title complexes exhibited good activities for ethylene polymerization (up to 1.56 × 106 g mol−1 (Ti) h−1). The C4/MMAO system was further investigated for the co-polymerization of ethylene with 1-hexene, 1-octene, or isoprene.