Ultrasonic nanocrystal surface modification (UNSM) is a unique, mechanical, impact-based surface severe plastic deformation (S2PD) method. This newly developed technique finds diverse applications in the aerospace, automotive, nuclear, biomedical, and chemical industries. The severe plastic deformation (SPD) during UNSM can generate gradient nanostructured surface (GNS) layers with remarkable mechanical properties. This review paper elucidates the current state-of-the-art UNSM technique on a broad range of engineering materials. This review also summarizes the effect of UNSM on different mechanical properties, such as fatigue, wear, and corrosion resistance. Furthermore, the effect of USNM on microstructure development and grain refinement is discussed. Finally, this study explores the applications of the UNSM process.