The inferior wear resistance of titanium alloys severely affects their lifespan. In this study, a novel method (referred to as CUSP) combining ultrasonic shot peening with TiN particles was explored, simultaneously preparing the TiN coatings and ultrafine-grained gradient structures on the surface of titanium alloys. The surface morphology and microstructure characteristics of the treated samples were examined, while the wear performance was evaluated using a friction and wear tester. The findings demonstrate that the CUSP-treated sample has a peak hardness of 581.6 HV, an elevation of 65.56 % and 31.94 % compared to the untreated (UT) and conventional ultrasonic shot-peened (USP) samples. The CUSP-treated sample exhibits excellent anti-wear properties, with a wear rate of only 5.82 × 10 −6 mm 3N −1 m −1, representing a reduction of 94.76 % and 93.91 % from that of the UT and USP samples, respectively. This improvement resulted from the synergistic effects of TiN coatings and ultrafine-grained gradient structures, which considerably alleviated the abrasive, fatigue, and adhesive wear. Additionally, the tribo-layer formed during wear served to isolate, load-bear, and provide solid lubrication effects, which further improve wear performance.