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Polyetheretherketone (PEEK) is growing in popularity for orthopedic, spinal, and trauma applications but has potential significant limitations in use. PEEK is biocompatible, similar in elasticity to bone, and radiolucent, but is inert and therefore does not integrate well with bone. Current efforts are focusing on increasing the bioactivity of PEEK with surface modifications to improve the bone-implant interface. We used a novel Accelerated Neutral Atom Beam (ANAB) technology to enhance the bioactivity of PEEK. Human osteoblast-like cells seeded on ANAB-treated PEEK result in significantly enhanced proliferation compared with control PEEK. Cells grown on ANAB-treated PEEK increase osteogenic expression of ALPL (1.98-fold, p < 0.002), RUNX2 (3.20-fold, p < 0.002), COL1A (1.94-fold, p < 0.015), IBSP (2.78-fold, p < 0.003), and BMP2 (1.89-fold, p < 0.004). Cells grown on these treated surfaces also lead to an increased mineralization (6.4-fold at 21 days, p < 0.0005). In an ovine study, ANAB-treated PEEK implants resulted in enhanced bone-in-contact by 3.09-fold (p < 0.014), increased push-out strength (control 1959 ± 1445 kPa; ANAB 4068 ± 1197 kPa, p < 0.05), and evidence of bone ingrowth at both the early (4 weeks) and later (12 weeks) time points. Taken together, these data suggest that ANAB treatment of PEEK has the potential to enhance its bioactivity, leading to bone formation and significantly decreasing osseointegration time of orthopedic and spinal implants. ANAB treatment, therefore, may significantly enhance the performance of PEEK medical implants and lead to improved clinical outcomes. © 2015 Wiley Periodicals, Inc. J Biomed Mater Res Part B: Appl Biomater, 105B: 531-543, 2017.