Structural and magnetic properties of Ni 81Fe 19/Zr multilayers, prepared by DC magnetron sputtering, were studied using X-ray diffraction, ferromagnetic resonance and magnetization. Low-angle X-ray diffraction results are typical of a modulated structure, while high-angle data suggest that the Ni 81Fe 19 layers can have amorphous or crystalline structure depending on the thickness. Saturation magnetization increases significantly with thickness of the Ni 81Fe 19 layers, an effect attributed to the increase in the bulk-to-interface ratio. In a sample where the thickness of the Ni 81Fe 19 layers is 40 Å, the FMR spectrum, with the magnetic field perpendicular to the film plane, displays a spin wave feature, with odd and even modes. Two surface modes are also observed, suggesting that unpinning occurs at both interfaces of the Ni 81Fe 19 layers. For Ni 81Fe 19 layers thicker than 40 Å, FMR and magnetization data show a surface anisotropy constant ( K S) of about −0.32 erg/cm 2, which is an indication that the magnetic moment in the Ni 81Fe 19 layers is confined to the film plane.