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Bacterial infection has become a crucial reason that give rise to failure of medical implants in clinical applications. In this regard, various antibacterial surface modifications of implants have been developed in recent years. However, it remains a challenge to enable the implant surfaces with both suitable antibacterial and osteogenic properties. In this work, ε-polylysine and gum Arabic multilayer composite films were immobilized layer by layer (LBL) on anodized titanium with the assistance of polydopamine for the first time. In vitro