Three metal (Ag, Cu, and Al) nanoparticle (NP) films are obtained by irradiating a smooth and continuous metal film with a Nd∶YAG fiber pulsed laser at room temperature. The tunability of the wavelength and intensity of localized surface plasmon resonance (LSPR) of the three metal NP films is realized by varying laser scanning speeds. The wavelength and intensity of the plasmon absorption peak of Ag NP film in visible wavelength region show a wide tuning range, while the wavelength and intensity of the plasmon absorption peak of the Cu NP film exhibit a small tuning range in the visible wavelength region. Unlike Ag and Cu NP films, the Al NP film exhibits a narrow and sharp plasmon absorption peak in the ultraviolet wavelength region, and the wavelength tuning range of LSPR is also small. Further, the stronger surface-enhanced Raman scattering signals are observed in all three kinds of laser-irradiated metal NP films than in the deposited metal films before laser irradiation. The results of the finite difference time-domain simulation with respect to the electric-field intensity distributions of all samples show good agreement with the experimental results of surface-enhanced Raman scattering.