Mica single crystal (001) surfaces are irradiated with light from an excimer laser (lambda=248 nm) and are analyzed via low-energy electron diffraction. It is shown that the excimer laser treatment makes them well suited for epitaxial growth of Au(lll) thin films (thickness 150-600 Angstrom). Further irradiation with the laser at reduced fluences improves the quality of the grown Au films significantly without the need for high-energy ion sputtering.