Laser ablation of Al-Ni alloys and multilayers has been studied by molecular dynamics simulations. The method was combined with a two-temperature model to describe the interaction between the laser beam, the electrons, and the atoms. As a first step, electronic parameters for the alloys had to be found and the model developed originally for pure metals had to be generalized to multilayers. The modifications were verified by computing melting depths and ablation thresholds for pure Al and Ni.Here known data could be reproduced. The improved model was applied to the alloys Al 3 Ni, AlNi and AlNi 3 . While melting depths and ablation thresholds for AlNi behave unspectacular, sharp drops at high fluences are observed for Al 3 Ni and AlNi 3 . In both cases, the reason is a change in ablation mechanism from phase explosion to vaporization. Furthermore, a phase transition occurs in Al 3 Ni. Finally, Al layers of various thicknesses on a Ni substrate have been simulated. Above threshold, 8 nm Al films are ablated as a whole while 24 nm Al films are only partially removed. Below threshold, alloying with a mixture gradient has been observed in the thin layer system.