Titanium and its alloys are widely used in blood contacting implantable and interventional medical devices; however, their biocompatibility is still facing great challenges. In this study, with the aim of improving the biocompatibility and antibacterial activities of titanium, TiO2 nanotubes with a diameter of about 30 nm were firstly prepared on the titanium surface by anodization, followed by the introduction of polyacrylic acid (PAA) and gentamicin (GS) on the nanotube surface by layer-by-layer method, and finally zinc ions were loaded into the surface to improve the bioactivities. The nanotubes have excellent hydrophilic properties and special nanotube-like structure, which can selectively promote the albumin adsorption and enhance the blood compatibility and promote the growth and functional expression of endothelial cells to a certain extent. After the introduction of PAA and GS, although the super-hydrophilicity cannot be achieved, the results of platelet adhesion, cGMP activity, hemolysis rate and partial thromboplastin time (APTT) showed that the blood compatibility was improved, and the blood compatibility was further enhanced after zinc ions loading on the surface. On the other hand, the surface modified materials showed good cytocompatibility to endothelial cells. The introduction of PAA and zinc ions not only promoted the adhesion and proliferation of endothelial cells, but also up-regulated expression of vascular endothelial growth factor (VEGF) and nitric oxide (NO). The slow and continuous release of GS and Zn2+ for more than 14 days, which can significantly improve the antibacterial properties of the materials. Therefore, the present study provides an effective method for the surface modification of titanium-based blood-contacting materials to simultaneously endow with good blood compatibility, endothelial growth behaviors and antibacterial properties.