In this research, four coatings including pure zinc, pure aluminum, a double-layered coating of zinc and aluminum, and a coating produced by simultaneous deposition of zinc and aluminum were deposited on a cast iron substrate using electric arc-spraying technique. The coatings were characterized by XRD, SEM and EDS map and spot analyses. Adhesion strength of the coatings was evaluated by three-point bending tests, where double-layered coating indicated the lowest bending angle among the specimens, with detection of cracks at the coating–substrate interface. Coatings produced by simultaneous deposition of zinc and aluminum possessed a relatively uniform distribution of both metals. In order to evaluate the corrosion behavior of the coatings, cyclic polarization and salt spray tests were conducted. Accordingly, pure aluminum coating showed susceptibility to pitting corrosion and other coatings underwent uniform corrosion. For double-layered coating, SEM micrographs revealed zinc corrosion products as flaky particles in the pores formed by pitting on the surface, an indication of penetration of corrosion products from the lower layer (zinc) to the top layer (aluminum). All coatings experienced higher negative corrosion potentials than the iron substrate, indicative of their sacrificial behavior.