Herein, amorphous silicon silver (a-Si∶Ag) thin films are prepared via magnetron co-sputtering and subjected to femtosecond laser irradiation. The scanning electron microscopy, Raman spectroscopy, integrating sphere, and semiconductor performance tester are used to characterize the surface morphology, microstructure, and photoelectric properties of thin films before and after irradiation. Results show that for an irradiation energy of 300 mJ/cm ², no obvious etching trace is observed on the surface of the a-Si∶Ag thin film, nanocrystalline Si particles are formed in the thin film, and the size of the Ag nanocrystals in the thin film increases. For an irradiation energy of 600 mJ/cm ², obvious etching marks appear on the surface of the thin film, and the size of the Ag nanocrystal increases; however, the nanocrystalline Si particles do not change in size. The a-Si∶Ag thin film irradiated by the femtosecond laser has low resistivity, and the irradiated film can diminish a reflection of the incident light in the visible-near-infrared band. The obtained results positively affect the performance of artificial synaptic devices based on a-Si∶Ag thin films.