Polyetheretherketone (PEEK) possesses a set of characteristics superior for biomedical applications including bone-like stiffness and suitable biocompatibility. However, the clinical adoption of PEEK as orthopedic and dental implants is severely hampered by its bioinert surface property. The present work aimed at tailoring the PEEK surface with –COOH, –OH and –PO4H2 functional groups for the enhancement of osteogenic activity. In vitro cell adhesion and viability analyses have clearly disclosed that enhanced adhesion, spreading and proliferation of MC3T3-E1 osteoblast on these functional groups modified PEEK surfaces. In vivo evaluation of the rat femur model by means of push-out tests and histological analysis after 4 and 12 weeks confirms improved osteointegration and bone-implant bonding strength. Preliminary results imply that an implant material tailored by –COOH, –OH or –PO4H2 functional groups on its surface has certain bioactivity. And the results may provide insight into the design of biomaterials with chemical functional groups for bone regeneration.