Bacteria killing behavior based on physical effects is preferred for biomedical implants because of the negligible associated side effects. However, our current understanding of the antibacterial activity of nanostructures remains limited and, in practice, nanoarchitectures that are created on orthopedics should also promote osteogenesis simultaneously. In this study, tilted and vertical nanolamellar structures are fabricated on semi-crystalline polyether-ether-ketone (PEEK) via argon plasma treatment with or without pre-annealing. The two types of nanolamellae can physically kill the bacteria that come into contact with them, but the antibacterial mechanisms between the two are different. Specifically, the sharp edges of the vertically aligned nanolamellae can penetrate and damage the bacterial membrane, whereas bacteria are stuck on the tilted nanostructures and are stretched, leading to eventual destruction. The tilted nanolamellae are more desirable than the vertically aligned ones from the perspective of peri-implant bone regeneration. Our study not only reveals the role of the arrangement of nanostructures in orthopedic applications but also provides new information about different mechanisms of physical antibacterial activity.