Ultrasonic nanocrystal surface modification (UNSM) technology was applied to the surfaces of specimens additively manufactured by powder bed fusion (PBF). The changes in roughness and hardness due to the UNSM were set as objective functions, and the optimal conditions for the main parameters were derived through the response surface method (RSM) and Box–Behnken design (BBD). Regression analysis-based mathematical models for predicting the surface hardness and roughness are presented and validated. The RSM results show that the surface roughness is highly dependent on the load and ball tip diameter, and the surface roughness significantly improves as the inter-pass interval and ball tip diameter decrease. Through BBD and ANOVA, the optimal conditions for the improvement of surface characteristics were found to be a load of 40 N, inter-pass interval of 10 μm, and ball tip diameter of 2.38 m. The surface treated under these optimal conditions exhibited a hardness of 497 Hv and surface roughness of 1.32 μm, which were significantly improved compared to the values for an untreated specimen. In addition, it was confirmed that the grains are significantly refined after UNSM, and scratch resistance increases for the top layer of the surface directly affected by the UNSM horn.
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