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Cancer cell targeted therapy using a biocompatible targeted drug delivery system can increase the therapeutic effects of cellular cancer therapy. Here, we report a Folic Acid (FA) and polyethyleneimine (PEI) functionalized Graphene Oxide (GO) nanocarrier, FA-PEI-GO, used to deliver two new Copper complexes into the folate-receptor-positive nasopharyngeal carcinoma cell line. GO was prepared by modified Hummers method and then decorated by PEI and FA. Afterwards, the material was characterized by the X-ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), and atomic force microscopy (AFM). Copper complexes were synthesized by a hydrothermal method and then characterized by single crystal X-ray diffraction analysis. Cytotoxicity assessment of the complexes illustrated that the IC50 values against the nasopharyngeal carcinoma cell lines, HNE-1 and CNE-2, were, respectively, 17.7 ± 1.2, 13.2 ± 1.9, 6.7 ± 0.8, 2.9 ± 0.7 μM. Flow cytometry findings suggested that both complexes were capable of decreasing cancer cell viability through causing late-stage cell apoptosis. The obtained targeted drug delivery systems had good biocompatibility and stability. Compared with Cis-Dichlorodiamineplatinum (CDDP), the non-specific antitumor drug normally used in chemotherapy, one of the obtained agents had similar therapeutic effect while the other had significantly higher activity, suggesting future possible application of this new targeted therapy against nasopharyngeal carcinoma.