It was demonstrated that the mechanical shot peening (MSP) technique was a viable way to obtain a nanocrystalline layer on a large size pure titanium plate due to the MSP provided for severe plastic deformation (SPD) of surface high velocity balls impacting. The MSP effects of various durations in producing the surface nanocrystalline layer was characterized by optical microscope (OM), X-ray diffraction (XRD), transmission electron microscope (TEM), and Vickers micro-hardness tester. The results showed that the thickness of the SPD layer gradually increased with the MSP processing time increase, but saturated at 230 μm after 30 min. The average grain size was refined to about 18.48 nm in the nanocrystalline layer. There was equiaxed grain morphology with random crystallographic orientation in the topmost surface. By comparing with the nanocrystalline layer, acquired by surface mechanical attrition treatment (SMAT), the microstructure and properties of the nanocrystalline layer acquired by MSP was evidently superior to that of the SMAT, but the production time was cut to about a quarter of the time used for the SMAT method.