The morphology and the spin-polarized electronic structure of the Fe 9 cluster supported on the (001) surface of Ni are investigated by combining the Modified Embedded Atom Model (MEAM) with quenched Molecular Dynamics (MD) and a selfconsistent non-collinear spd Tight-Binding (TB) method parameterized to ab-initio Tight-Binding Linear Muffin-Tin Orbital (TB-LMTO) results. Two-dimensional geometry and overall ferromagnetic coupling are found, in keeping with recent experimental findings. The local magnetic moments and Fe–Ni hybridization effects are analyzed in terms of the interfacial relaxation.