Poly(etheretherketone) exhibits good biocompatibility, excellent mechanical properties, and bone-like stiffness. However, the natural bio-inertness of pure poly(etheretherketone) hinders its applications in biomedical field, especially when direct bone-implant osteo-integration is desired. For developing an alternative biomaterial for load-bearing orthopedic application, combination of bioactive fillers with poly(etheretherketone) matrix is a feasible approach. In this study, a bioactive multi-walled carbon nanotubes/calcium polyphosphate/poly(etheretherketone) composite was prepared through a compounding and injection-molding process for the first time. Bioactive calcium polyphosphate was added to polymer matrix to enhance the bioactivity of the composite, and incorporation of multi-walled carbon nanotubes to composite was aimed to improve both the mechanical property and biocompatibility. Furthermore, the microstructures, surface hydrophilicity, and mechanical property of multi-walled carbon nanotubes/calcium polyphosphate/poly(etheretherketone) composite, as well as the cellular responses of MC3T3-E1 osteoblast cells to this material were investigated. The mechanical testing revealed that mechanical performance of the resulting ternary composite was significantly enhanced by adding the multi-walled carbon nanotubes and the mechanical values obtained were close to or higher than those of human cortical bone. More importantly, cell culture tests showed that initial cell adhesion, cell viability, and osteogenic differentiation of MC3T3-E1 cells were significantly promoted on the multi-walled carbon nanotubes/calcium polyphosphate/poly(etheretherketone) composite. Accordingly, the multi-walled carbon nanotubes/calcium polyphosphate/poly(etheretherketone) composite may be used as a promising bone repair material in dental and orthopedic applications.