Crystallization from an amorphous atomic structure is usually seen as a spontaneous process in pursuit of a lower energy state, but for alloy systems it is often hard to elucidate because of the intrinsic structural and compositional complexity. Here, by means of electron beam irradiation, we found surface-limited, and thus size-dependent crystallization in a system of monoatomic Pd metallic glass, which is ascribed to the structural differences between the surface and the interior. The equilibrium thickness of the surface crystallization is controllable, presenting a promising approach to fabricate novel nanostructures. The investigation is believed to provide a general understanding of solid amorphous-to-crystalline phase transition from the nanoscale to the bulk size.