Silver, known for its high thermal and electrical conductivity, is an ideal metal for thin-film electrode applications. Because alloying can negatively affect conductivity, enhancing the strength and resistance to strain poses a tremendous challenge when applied to pure Ag films. Herein, in both experiments and atomistic simulations, we discover a nanoscale strengthening mechanism by intercalating ultrathin amorphous Ni-rich layers between pure nanocrystalline Ag films, resulting in the formation of a multilayered Ag and Ni-Ag alloy material with a stable grain size (22 nm) combining the highest hardness (2.6 GPa), tensile strength (677 MPa) and plastic elongation (6.6%) ever reported for this metal. The integration of amorphous Ni-Ag alloy nanolayers substantially improves the strain hardening behavior and extends the tensile ductility compared to standard crystalline Ag/Ni nanolaminates at an equivalent Ag layer thickness. This phenomenon results from strain-induced chemical short-range order within the amorphous Ni-Ag nanolayers during plastic deformation. The new nanoscale strengthening mechanism can be easily leveraged to develop nanocrystalline films with exceptional mechanical and physical properties.