To improve the microstructure compactness and wear resistance of the micro-arc oxidation (MAO) coating on the surface of TC21 alloy, a laser remelting modification was performed on the surface of the MAO coating. The microstructure, composition, phase composition, hardness, friction, and wear properties of the remelted coating were characterized. The results show that the laser remelted coating consists of three layers: outer layer, inner layer, and heat-affected layer, of which the outer and inner layer is mainly composed of Al2TiO5, rutile-TiO2 and α-Al2O3, and the heat affected layer is mainly composed of α-Ti and the transformed β phases. The hardness of the remelted MAO coating increases significantly. The friction coefficient of the remelted coating is lower than MAO coating and TC21 substrate in the wear test. The wear mechanism of remelted coating is adhesive wear, accompanied by slight abrasive wear. Laser remelting MAO coating significantly improved the friction and wear properties of TC21 titanium alloy.