A nanocrystalline-amorphous (NC-A) mixed layer was obtained by ultrasonic shot peening (USP) on pure titanium at room temperature and observed by X-ray diffraction pattern (XRD), scanning electron microscope (SEM) and high-resolution transmission electron microscope (HRTEM). The results showed that the amorphization percentage in the NC-A mixed layer increased continuously with the increase of the peening duration, shot diameter and sonotrode amplitude or the decrease of the peening distance. The maximum amorphization percentage achieved in this study was 44.09%. Moreover, with the amorphization percentage in the NC-A mixed layer increasing, the surface hardness increased constantly. Base on the experimental results, the amorphization mechanism during USP treatment was also analyzed.