Amorphous coating technology is an attractive way of taking advantage of the superior properties of amorphous alloys for structural applications. However, the limited bonds between splats within the plasma-sprayed coatings result in a typically lamellar and porous coating structure. To overcome these limitations, the as-sprayed coating was treated by a laser-remelting process. The microstructure and phase composition of two coatings were analyzed using scanning electron microscopy with energy-dispersive spectroscopy, transmission electron microscopy, and x-ray diffraction. The wear resistance of the plasma-sprayed coating and laser-remelted coating was studied comparatively using a pin-on-disc wear test under dry friction conditions. It was revealed that the laser-remelted coating exhibited better wear resistance because of its defect-free and amorphous-nanocrystalline composited structure.