Abstract. In the present study, a polyethylene terephthalate (PET) artificial ligament was coated with an organic layer-by-layer (LBL) self-assembled template of chitosan and hyaluronic acid, and then incubated in a calcium phosphate (CaP) solution to prepare a biomimetic CaP coating. The surface characterization of the ligament was examined using scanning electron microscopy, atomic force microscopy and energy-dispersive X-ray spectroscopy. The effects of CaP coatings on the osteogenic activity of MC3T3 E1 mouse osteoblastic cells were investigated by evaluating their attachment, proliferation and the relative expression levels of alkaline phosphatase. The results revealed that the organic LBL template on the PET artificial ligament was effective for CaP apatite formation. Following incubation for 72 h, numerous nanoscale CaP apatites were deposited on the PET ligament fibers. In addition, the results of the in vitro culture of MC3T3-E1 mouse osteoblastic cells demonstrated that the CaP coating had a good biocompatibility for cell proliferation and adhesion, and the CaP-coated group had a significantly higher alkaline phosphatase activity compared with the uncoated control group after seven days of cell culture. Collectively, these results demonstrated that the biomimetic nanoscale CaP-coated PET artificial ligaments have potential in bone-tissue engineering.