Additive manufacturing enables the fabrication of patient-specific implants of complex geometries. Although selective laser melting (SLM) of 316L stainless steel (SS) is well established, post-processing is essential to preparing high-performance biomedical implants. The goal of this study was to investigate surface mechanical attrition treatment (SMAT) as a means to enhance the electrochemical, biomechanical, and biological performances of 316L SS fabricated by SLM in devices for the repair of bone tissues. The SMAT conditions were optimized to induce surface nanocrystallization on the additively manufactured samples. SMAT resulted in a thicker oxide layer, which provided corrosion resistance by forming a passive layer. The fretting wear results showed that the rate of wear decreased after SMAT owing to the formation of a harder nanostructured layer. Surface modification of the alloy by SMAT enhanced its ability to support the attachment and proliferation of pre-osteoblasts in vitro. The study of the response in vivo to the additively manufactured alloy in a critical-sized cranial defect murine model revealed enhanced interactions with the cellular components after the alloy was subjected to SMAT without inducing any adverse immune response. Taken together, the results of this work establish SMAT of additively manufactured metallic implants as an effective strategy for engineering next-generation, high-performance medical devices for orthopedics and craniomaxillofacial applications.