The paper reviews the results of investigations of surface modification and alloying of Al, Ti, and its alloys with a low-energy (up to ∼40 keV), high-current (up to 25 J/cm 2 ) electron beams of microsecond duration under systematically varied conditions. The microstructural evolution of the surface layers of Al alloys (Al2024 and Al6061) and Ti-6Al-4V alloy subjected to pulsed melting as well as changes in surface-sensitive properties of these alloys are considered. Phase formation and properties of Albased and Ti-based surface alloys, synthesized by liquid-phase mixing of multilayer film-substrate systems in wide range of solid solubility, including [Al/Si]/Al, [Al/C]/Al, [Zr/Ti]/Ti-6Al-4V, and Al/Ti, are studied. In case of Ti-based substrates, this method allows to fabricate the single-phase nanocrystalline α-(TiZr) surface alloy, free of Al and V, as well as nanosized and ultrafine grain TiAl/Ti 3 Al-based surface alloys of thickness ≥3 μm with enhanced mechanical properties.