Diverse metallic parts should have high wear resistance. Therefore, to achieve an ultrawear-resistant surfacefor cast iron, we developed a new process that combines stick burnishing with ultrasonic nanocrystal surfacemodification (UNSM). Stick burnishing is a well-known process that creates a compressive residual stressthrough a work-hardening effect. The UNSM treatment refined the grain structure to increase the hardnessand compressive residual stress. In this study, four types of specimens, UNSM alone and burnishing alone,and two combined treatments, UNSM-after-burnishing and burnishing-after-UNSM, were sequentially evaluated,and their surface hardness distributions were compared. This operation resulted in the best combination ofmechanical surface treatments, the hardness was found to be 61.4% higher than that of the original cast ironmaterial. We believe that this approach can be applied to a variety of mechanical components for highlyfunctional local surface properties and ultra-wear resistance applications.