The interplay between atomic geometry and magnetic properties of Fe atoms at the Fe-Ni(1 1 1) interface was studied. To this end dichroic optical absorption and reflectivity (both in energy and theta -2 theta angular scan mode) were carried out in the L-2,L-3 edge region of Fe in (Fe-6 (Angstrom)/Ni-24 (Angstrom)(1 1 1))(10) multilayer while the atomic geometry of the Fe site at the interface was studied for 1 atomic layer of Fe on Ni(1 1 1) by photo-electron diffraction tin angular scan mode and back-scattering regime). The Fe atom was found to be chemisorbed in an fee hollow site and to stack pseudomorphically to Ni(1 1 1). Its magnetic moment was found to be in the range 2.9 +/-0.9-1.93 +/- 0.6 mu (B). Possibility of surface anisotropy is discussed.