Ultrafine-grained pure titanium prepared by equal-channel angular pressing has favorable mechanical performance and does not contain alloy elements that are toxic to the human body. It has potential clinical value in applications such as cardiac valve prostheses, vascular stents, and hip prostheses. To overcome the material’s inherent thrombogenicity, surface-coating modification is a crucial pathway to enhancing blood compatibility. An electrolyte solution of sodium silicate + sodium polyphosphate + calcium acetate and the micro-arc oxidation (MAO) technique were employed for in situ oxidation of an ultrafine-grained pure titanium surface. A porous coating with anatase- and rutile-phase TiO2 was generated and wettability and blood compatibility were examined. The results showed that, in comparison with ultrafine-grained pure titanium substrate, the MAO coating had a rougher surface, smaller contact angles for distilled water and higher surface energy. MAO modification effectively reduced the hemolysis rate; extended the dynamic coagulation time, prothrombin time (PT), and activated partial thromboplastin time (APTT); reduced the amount of platelet adhesion and the degree of deformation; and enhanced blood compatibility. In particular, the sample with an oxidation time of 9 min possessed the highest surface energy, largest PT and APTT values, smallest hemolysis rate, less platelet adhesion, a lesser degree of deformation, and more favorable blood compatibility. The MAO method can significantly enhance the blood compatibility of ultrafine-grained pure titanium, increasing its potential for practical applications.