The results of experimental investigations of microstructure and phase composition of surface ion-alloyed layers of nickel, titanium, and iron formed under the conditions of high-intensity aluminum-ion implantation are presented. It is established that aluminum-ion implantation under high-intensity modes makes it possible to form finely-dispersed intermetallic phases of Me3Al (Me = Ni, Ti, Fe) and MeAl (Ni, Ti), as well as solid solutions of a composition variable with respect to depth in the surface layers measuring up to 2000 nm. It is shown that the average grain-size of intermetallic phases formed in ion-alloyed layers is 20–80 nm. Regions of localization of the phases thus formed over the implanted layer depth are determined.