Ultrathin films of bcc Fe (001) on Ag (001) and Fe/Ni (001) bilayers on Ag were grown by molecular beam epitaxy. A wide range of surface science tools (RHEED, REELFS, AES, and XPS) were employed to establish the quality of epitaxial growth. Ferromagnetic resonance and Brillouin light scattering were used to extract the magnetic properties. Emphasis was placed on the study of magnetic anisotropies. Large uniaxial anisotropies with the easy axis perpendicular to the film surface were observed in all ultrathin structures studied. In sufficiently thin samples the saturation magnetization was oriented perpendicular to the film surface in the absence of an applied field. It has been demonstrated that in bcc Fe films the uniaxial perpendicular anisotropy originates at the film interfaces. Fe/Ni bilayers were also investigated. Ni grows in the pure bcc structure for the first 3–6ML and then transforms to a new structure which exhibits unique magnetic properties. Transformed ultrathin bilayers possesses large in-plane 4th order anisotropies far surpassing those observed in bulk Fe and Ni. The large 4th order anisotropies originate in crystallographic defects formed during the Ni lattice transformation.