Chemo-sensitization therapy has gained importance in the field of anti-cancer treatment in recent years. The combination of both chemotherapy and chemosensitization has unique advantages. However, there has been relatively limited research on combination treatment using metal complexes and chemosensitizers. Herein, we reports a two-drug synergistic delivery system combining a copper complex and a chemosensitizer Olaparib in a certain ratio of safety and efficiency is the key. Polyethylenimine (PEI) was chemically-linked to activated chemosensitizer Olaparib, which was connected to a bifunctional peptide, T15, for facilitation and nuclear targeting, resulting in Ola-PEI-T15. Then, a novel metal complex Cu/Ola-PEI-T15 was obtained by Cu 2+ coordination to Ola-PEI-T15. The two therapeutic agents can be transported into the cells at the same time, giving full play to the synergistic anti-tumor effect.