High-quality thin-film superlattices of permalloy (NiFe) and silver (Ag) have been grown by pulsed laser deposition (PLD) for the first time. The alternating metallic layers weregrown from individual NiFe and Ag targets utilizing an automated multi-target holder coupled to a conventional PLD system. The targets were ablated at a base pressure of 4×10−7 Torr and the material deposited on room-temperature (100) silicon and on fused silica substrates. The films were characterized by X-ray diffraction (XRD), magnetic field-dependent resistivity, and ferromagnetic resonance (FMR). XRD was used to confirm uniform bilayer thicknesses. The magnetic field-dependent resistance measurements indicated the presence of magnetoresistance in the deposited films. An as-deposited film with a bilayer thickness of 75 Å demonstrated a roomtemperature magnetoresistive effect of 0.15 %. FMR has been used to determine the relationship between NiFe magnetism and the observed magnetoresistance.