The AZ91 magnesium alloy was subjected to a complex treatment involving age hardening (supersaturation and artificial aging) and simultaneous surface layer modification. The specimens were supersaturated in contact with a mixture containing varying concentrations of zinc chloride, followed by cooling either in air or water. After supersaturation, the specimens were subjected to artificial aging and then air-cooled. This process resulted in the formation of a surface layer made of zinc-rich phases. The thickness and microstructure of the surface layer were influenced by the process parameters, namely, the zinc chloride content in the mixture and the cooling rate during supersaturation. The treated specimens exhibited favorable tensile strength and greater elongation compared to the as-cast AZ91 alloy, with values comparable to those of the alloy subjected to standard T6 tempering. No cracking of the layer was observed under moderate deformation, though greater deformation resulted in the formation of cracks, primarily in the areas containing the Mg5Al2Zn2 intermetallic phase. The produced layer demonstrated strong metallurgical bonding to the AZ91 substrate.