Silver nanostructured thin films have been fabricated on silicon substrate by combining simultaneously pulsed laser ablation in liquid (PLAL) and electrophoretic deposition (ED) techniques. The composition, topography, crystalline structure, surface topography, and optical properties of the obtained films have been studied by energy dispersive X-ray spectroscopy (EDS), high-resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD), and UV-visible spectrophotometry. The coatings were composed of Ag nanoparticles ranging from a few to hundred nm. The films exhibited homogenous morphology, uniform appearance, and a clear localized surface plasmon resonance (LSPR) around 400 nm.