Thin films of Cu on Zr and of Zr on Fe, Ni, Al, V, and Ti have been laser-pulse alloyed with the substrate metals using a raster-scanned Q-switched Nd:YAG laser. The high quench rates from the liquid state attendant to laser-pulse melting can promote the retention of a variety of metastable alloy phases. Structure and composition of the surface alloy layers of submicron thickness were studied with Rutherford backscattering (RBS)/channeling spectroscopy, optical and transmission electron microscopy and glancing angle x-ray diffraction (XRD). Composition profiles are compared with expected liquid-state diffusivities and structures are related to properties of bulk alloys. For example, in the well-known glass-forming system Cu-Zr, an amorphous phase was formed which crystallized upon annealing above Tc. In the Zr-Ti system, which shows complete solid solubility across the binary phase diagram in both the α and β phases, the hexagonal α-phase alloy is formed. Additional results on these and other systems are described below.