Phase composition, structural state, and mechanical properties of the ion-doped surface layers of Ni, Ti, and Fe targets with Al and Ti ions implanted into using the metal ion beam and plasma source Raduga 5 have been investigated. The high-intensity mode of implantation allowed us to obtain the ion-doped layers with the thickness exceeding the ion projected range by several orders of magnitude. By the transmission electron microscopy, it has been found that the fine-dispersed equilibrium intermetallic phases (Me3Al, MeAl) and the solid solution of aluminum were formed in the doped Ni, Ti, and Fe surface layers at the depth of up to 2600 nm. The maximum dopant concentration reached 75%. It has been shown that the average size of the formed phases was of 70 nm. The microhardness of the different target surface layers increased by 1.5–3 times. The wear resistance of the samples did not change within the temperature range of 300–700 K.