Gradient structured materials possess good combinations of strength and ductility, rendering the materials attractive in industrial applications. In this research, a surface nanocrystallization (SNC) technique, rotationally accelerated shot peening (RASP), was employed to produce a gradient nanostructured pure Ti with a deformation layer that had a thickness of 2000 μm, which is thicker than those processed by conventional SNC techniques. It is possible to fabricate a gradient structured Ti workpiece without delamination. Moreover, based on the microstructural features, the microstructure of the processed sample can be classified into three regions, from the center to the surface of the RASP-processed sample: (1) a twinning-dominated core region; (2) a “twin intersection”-dominated twin transition region; and (3) the nanostructured region, featuring nanograins. A microhardness gradient was detected from the RASP-processed Ti. The surface hardness was more than twice that of the annealed Ti sample. The RASP-processed Ti sample exhibited a good combination of yield strength and uniform elongation, which may be attributed to the high density of deformation twins and a strong back stress effect.