The mechanisms of femtosecond laser-induced transient melting and atomic mixing in a target composed of a 30 nm Au film deposited on a bulk Cu substrate are investigated in a series of atomistic simulations. The relative strength and the electron temperature dependence of the electron-phonon coupling of the metals composing the layered target are identified as major factors affecting the initial energy redistribution and the location of the region(s) undergoing transient melting and resolidification. The higher strength of the electron-phonon coupling in Cu, as compared to Au, results in a preferential sub-surface heating and melting of the Cu substrate, while the overlaying Au film largely retains its original crystalline structure. The large difference in the atomic mobility in the transiently melted and crystalline regions of the target makes it possible to connect the final distributions of the components in the resolidified targets to the history of the laser-induced melting process, thus allowing for experimental verification of the computational predictions. (C) 2009 Elsevier B. V. All rights reserved.