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The neodymium chloride complex [Nd(ONN'O)Cl(THF)]2 supported by amine-bis(phenolate) ligand was synthesized by the metathesis reaction of anhydrous NdCl3 with Li2(ONN'O) [H2ONN'O = Me2NCH2CH2N(CH2-3-But2-5-Me-C6H2OH)2] in high yield. X-ray structural determination shows [Nd(ONN'O)Cl(THF)]2 complex consists of two seven-coordinate neodymium centers linked through μ-Cl bridges. And this complex was successfully used to initiate the ring-opening polymerization (ROP) of ε-caprolactone.