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An Fe-based amorphous coating, with the composition Fe₄₈Cr₁₅Mo₁₄C₁₅B₆Y₂, was synthesized by the high-velocity oxygen fuel spray (HVOF) process on a substrate of AISI 1035. The effect of crystallization on the electrochemical and tribological properties of the HVOF-sprayed Fe-based coating was systematically studied. The XRD results validated the fully amorphous nature of the as-sprayed coating by showing a broad peak at 43.44° and crystallization of this coating after heat-treatment at 700 °C by demonstrating sharp peaks of Fe-, Mo-, and Cr-based carbides. After crystallization, an increase in the corrosion current density from 4.95 μAcm⁻² to 11.57 μAcm⁻² and in the corrosion rate from 4.28 mpy to 9.99 mpy, as well as a decrease in the polarization resistance from 120 Ωcm² to 65.12 Ωcm², were observed, indicating the deterioration of the corrosion resistance of the as-sprayed Fe-based coating. This can be attributed to the formation of porous ferrous oxide, providing an easy channel for charge transfer and promoting pit formation. However, a decrease in the coefficient of friction from 0.1 to 0.05 was observed, highlighting the significant improvement in the wear resistance of the Fe-based coating after crystallization. This can be associated with the precipitation of hard carbides (MxCy) at the boundaries of the crystallized regions.