Surface mechanical attrition treatment (SMAT) was used to fabricate nanocrystalline surface layers on the commercial purity titanium. X-ray diffraction and transmission electron microscopy results indicate that the top layer contained nanograins. Enhanced strength and microhardness were achieved due to the surface nanostructure. Cell culture tests have shown a greater adhered cell density and more extensively spreading morphologies of Saos-2 cells on the SMAT substrates compared to those on the as-received Ti counterparts. Enhanced cell viability and cell cycle were also achieved on the SMAT Ti substrates. These could be attributed to the nanostructure grains with the increased surface hydrophilicity and roughness on the SMAT Ti.