This paper reports on a phenomenon associated with high-current pulsed electron beam (HCPEB) treatment: surface nanocrystallization of coarse primary phase in hypereutectic Al17.5Si and quasicrystal alloys after multiple pulses of HCPEB irradiation. The HCPEB treatment induces superfast heating and diffusion of alloying elements and heterogeneous nucleation in a melting solution, followed by rapid solidification and cooling of the material surfaces. Consequently, nanostructured surface layers can be achieved easily. Nano-Si phase and nano-quasicrystal phase formation on the modified surface layer of hypereutectic Al17.5Si alloy and quasicrystal alloy (Mg37Zn60Y3) show a potential for surface nanocrystallization of materials with enhanced properties by HCPEB treatment.