We report the results of continuous wave laser interactions with both gold and silver targets in the presence of different liquids (deionized water, ethanol, and glycerol). Upon moderate laser irradiation at wavelength of 1.06 nm during 30 min, nanoparticle colloids are shown to be formed with surprisingly narrow size distributions and average dispersion as small as 15–20 nm. The average particle sizes range between 8 and 52 nm for gold and between 20 and 107 nm for silver. This parameter is shown to be stable and well-controlled by such laser parameters as intensity and effective irradiation time, as well as by the choice of the liquid phase. The possibilities of an efficient control over the proposed synthesis techniques are discussed, and the results of a bimetallic Au–Ag structure deposition from the obtained colloids are presented. The formation of the extended arrays of gold and silver nanoparticles with controlled morphology is examined. The changes in the optical properties of the obtained thin films are found to depend on their morphology, in particular, on the particle size, and distance between them.