Al-based MIL-53 MOF nanostructure was synthesized hydrothermally and then co-deposited in the electroless nickel coating on AM60B magnesium alloy using Zr pretreatment as an eco-friendly underlayer. The MIL-53(Al) nanostructure was synthesized in the form of layered semi-cube crystals with the surface area and mean pore diameter of 985.72 m 2 g −1 and 2.00 nm, respectively. The SEM images captured with two various zooming scales from the surface of the plain and MOF containing electroless layers showed cauliflower-like morphology with even distribution of nodule size. Also, the sub-grains of the plain coating disappeared after incorporation of the MOF. Although, both the normal and nanostructure-containing electroless layers have crystalline-amorphous structure, but the nanocomposite coating showed less crystallinity. The average surface roughness of the plain electroless coating was about 309 nm, which decreased to about 222 nm after incorporation of the MOF. The XRD patterns showed that the characteristic peak of Ni broadened after incorporation of the MOF, probably due to the decreasing of the crystallinity. For the heat-treated normal and MOF containing coatings at 200 °C no phase transition takes place, but new peaks appeared for heat-treated coatings at 400 °C due to the crystallization and second-phase precipitation. The results of the EIS tests showed an increase in the amount of the charge transfer resistance (from 19 to 29 kΩ cm 2 ) after addition of the MOF, which means an improvement in the corrosion resistance. Also, low J corr of the composite coating represents its higher corrosion resistance with respect to the plain coating. The micro-hardness values of the composite coating before and after the heat treatment were higher than the plain coating. Also, the Ni-P-MOF coating has a lower wear rate both before and after the heat treatment due to an improvement in its micro-hardness.