TC21 titanium alloy possesses the advantage including high strength, low density, and great resistance to damage. Combining it with surface modification technology, it is expected to improve the performance of aviation structural components. This work applied laser remelting technology to realize surface modification, and the hardness and fretting wear properties of the coating were investigated. This research has found that laser remelting technology can effectively refine grain size and improve the performance of coatings. By exploring different laser remelting powers (600 W, 900 W, 1200 W) and the different diameters of laser beam (3 mm, 6 mm), the optimal laser process was obtained with laser power and spot diameter of 600 W and 6 mm, respectively. The average grain size is 2.1 μm. The laser remelting coating has an average microhardness about 980 HV0.2, and it is 2.5 times and 1.3 times higher than the substrate and laser cladding hardness, respectively. A minimum coefficient of friction (COF) about 0.5 was obtained by the laser remelting coating, and the wear rate reaches the lowest of 1.87 × 10−6 mm3/(N·m) at fretting temperature with 500 °C. The abrasive wear and adhesive wear were the main wear mechanisms, and accompanied by oxidative wear. This study provides important reference for improving the performance of high-strength titanium alloy to obtain low defect, high-performance coatings with stable quality.