This study aims to explore the effects of ultrasonic impact parameters on the surface modification of a stainless steel coating deposited on a medium-carbon low-alloy steel using argon arc surfacing welding. Ultrasonic impact treatment (UIT), at three different vibration strike numbers (40,000 times/(mm2), 57,600 times/(mm2), and 75,000 times/(mm2)) marked UIT–1, UIT–2, and UIT–3, respectively, was carried out to modify the surface structure and properties of the stainless steel coating. The surface morphological and structural features, phase compositions, grain size, topography, micro-mechanical properties, as well as the wear resistance of the coating before and after UIT with different impact parameters were experimentally investigated. The results of optical microscopy (OM), scanning electron microscopy (SEM), electron backscatter diffraction (EBSD), and X-ray diffraction (XRD) analyses revealed that the grain refinement accompanied by the formation of the strain-induced α′–martensite occurred on the UIT-treated coating surface. With the increase in the vibration strike number, the surface grain size and roughness decreased, while the α′–martensite content increased. Micro-hardness after UIT was increased by about 19% (UIT–1), 39% (UIT–2), and 57% (UIT–3), and the corresponding wear rate obtained was decreased by 39%, 72%, and 85%, respectively. Significant improvements in wear resistance were achieved using UIT. However, an excessive vibration strike number on the per unit area (/mm2) might result in unwanted micro-cracks and delamination on the treated surface, deteriorating the performance of the coating. These findings validate that UIT parameters (such as the vibration strike number on per unit area) are of great importance to bringing about improvements in wear performance, and UIT is found to have a high potential in modifying the surface characteristics and optimizing the mechanical performances of the deposited coating for a wide range of potential applications.