Adhesion of regenerating bone tissue to orthopaedic implants is critical to their long‐term success. Titanium has excess rigidity, interferes with imaging, and complicates radiation treatment. Poly(ether‐ether‐ketone) (PEEK) is a preferred material, but is limited by biological inertness. We show that plasma immersion ion implantation (PIII) imparts osteoadhesion on 3D printed PEEK using in vitro pull‐off tests and in vivo torque tests in a sheep scapula model. PIII‐PEEK prints incubated with bone cells in vitro show 9–14 times higher pull‐off strength, compared to untreated implants. Treated implants in vivo require seven times higher torque for release from the sheep scapula. We propose PIII‐PEEK as a scaffold material with tensile properties analogous to collagen, the fibrillar component of bone, to produce fracture‐tough fully integrating scaffolds.