The surfaces of nano-calcium silicate (n-CS)/polyetheretherketone (PK) composites were treated with abrasive paper and sand-blasting, and the surfaces performances of the as-treated composites were studied. The results showed that the surface roughness, hydrophilicity and mineralization of the simulated body fluid (SBF) of the composites surfaces were significantly improved, and the properties of the composites treated by with sand-blasting were better than those treated with abrasive paper. Moreover, the treated composites significantly promoted osteoblasts responses, such as cell attachment, spreading, proliferation and alkaline phosphatase (ALP) activity, compared to un-treated composites, and the cellular responses to the composites treated with sand-blasting were better than those treated with abrasive paper. The results suggested that surface treatment with sand-blasting was an effective method to greatly improve the surface bioperformances of the n-CS/PK composite, and this treated composite with improved bioactivity and cytocompatibility might be a promising implant material for orthopedic applications.