Fe-based amorphous composite coating was deposited on the carbon steel substrate by arc spraying and then remelted by a plasma remelting system, in order to improve the mechanical properties of the coatings. The composition, microstructure, and properties of the composite coating were analyzed by means of the metallographic microscope, scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), X-ray diffraction (XRD), and microhardness tester. The results showed that the amorphous composite coatings had more homogeneous and finer microstructure after the plasma remelting. The coating is metallurgically bonded with the substrate, and the hardness of the Fe-based amorphous composite coating is up to 1220 HV. The internal relationship between microhardness and microstructure has been discussed.