Herein, Ag-Mo films were deposited on Si(100) substrates by magnetron co-sputtering. The phase evolution and microstructural investigation revealed that the pure Ag phase and no Ag(Mo) solid solution were formed in the Ag-rich films even though the Mo content reached 53 at.%. However, the metastable Mo(Ag) solid solution was formed on the Mo-rich side. The Young's modulus, hardness, resistivity and the relationship between these properties and the microstructural evolution of Ag-Mo films were studied. Precisely, when the Mo content was controlled at 86 at.%, the hardness reached the maximum value of 14.64 GPa, and exceeded that of the pure Mo film. Meanwhile, the resistivity appeared to be a minimum value because the film had the maximum solid solubility and better crystallinity. The study on the microstructural, mechanical and electrical properties of Ag-Mo films provided a basis for the application of the film in electrical contact coatings.