Moving nanosecond laser system is used for laser-assisted thermodiffusion deposition of metallic nanoparticles from water-based colloidal solutions. The results obtained for both gold and silver nanoparticles show that film morphology strongly depends on laser scanning speed and the number of passages. We show, furthermore, the possibility of producing bimetallic Au:Ag thin films by laser irradiation of the mixed solutions. As a result of several laser scans, granular nanometric films are found to grow with a well-controlled composition, thickness, and morphology. By changing laser scanning parameters, film morphology can be varied from island structures to quasi-periodic arrays. The optical properties of the deposited structures are found to depend on the film composition, thickness, and mean separation between the particles. The transparency spectra of the deposited films are shown to be defined by their morphology.