To further improve the hemocompatibility of titanium (Ti) biomaterials, a bioactive coating was prepared by self-assembly of phase-transited lysozyme (PTL) and heparin (Hep). Scanning electron microscopy (SEM), atomic force microscopy (AFM), X-ray photoelectron spectroscopy (XPS), and water contact angle (WCA) measurement systematically confirmed the successful preparation of PTL/Hep coating on pure Ti surfaces. Blood compatibility assays showed that the platelet-repellent effect of the coating was significantly better than that of pure Ti surfaces. Also, the coating significantly extended the blood clotting time to 40.8 min. Besides, the hemolysis rate of PTL/Hep coated Ti substrates was only 0.39 ± 0.13%. These results confirmed the exceedingly excellent blood-compatibility of Ti surfaces modified by the self-assembled PTL/Hep coating.