The Fe/Zr composite coating was prepared by duplex Fe/Zr ion implantation and deposition to modify the microstructure and corrosion behavior of Mg-5.5 Zn-0.6 Zr (in wt.%, ZK60) alloy. The surface and interface characteristics were investigated using X-ray diffraction (XRD), atomic force microscope (AFM) and scanning electron microscopy (SEM). The results showed that the Fe/Zr composite coating exhibited a bi-layer microstructure of outer Fe-rich layer and inner Zr-rich layer. Multi-phases of α-Fe, ZrO0.35 and Zr6Fe3O were formed on the modified surface. The electrochemical measurements and immersion tests revealed an improvement of corrosion behavior for the surface-modified sample due to the protective effect of Fe/Zr composite coating.