Fe films 2–20 atomic monolayers (ML) thick have been deposited on Ni(1 1 1) films (4–60 ML) prepared on W(1 1 0) under UHV conditions. The Ni(1 1 1) films grow in a Nishijama–Wassermann orientation with a 3.6% lattice expansion along Ni[2̄ 1 1] (‖ W[1̄ 1 0]). On top of these slightly distorted Ni films iron is observed to grow preferentially in two mirror orientations. The saturation magnetization of these Fe films and the anisotropies of Fe/Ni bilayers have been studied using torsion oscillation magnetometry. The magnetization of the Fe films of 2.13 μ B per atom is close to the bulk value of Fe. The out-of-plane surface (interface) anisotropy constant K FeNi s=(−0.65±0.15) mJ/m 2 of the bilayers prefers a magnetization perpendicular to the surface. The exceptionally high value of the volume anisotropy constant of the Fe films, K Fe v=(+0.71±0.10) MJ/m 3=(52.2±7.5) μeV/atom, was ascribed to magnetoelastic contributions.