Synthesis of high SFE nanotwinned metallic films with varying distributions of twin widths on a low SFE metallic layer using magnetron sputtering is disclosed. In various embodiments, a method for forming a nanotwinned metal film may include providing a single crystal silicon wafer, etching the single crystal silicon wafer, depositing a silver film onto the single crystal silicon wafer forming a silver buffer layer, and depositing a metallic film onto the silver buffer layer using sputtering at a controlled temperature.