Gold particles were fabricated by the high-intensity femtosecond laser irradiation of gold (III) chloride trihydrate (HAuCl4) aqueous solution. The structure and size distribution of the prepared particles were evaluated by transmission electron microscopy. The configuration of the gold particles varied with the concentration of the HAuCl4 aqueous solution. The mean particle size and size distribution were changed by the addition of polyvinylpyrrolidone (PVP), which acted as a dispersant, and monodispersed gold nanoparticles with a diameter of about 3 nm were successfully fabricated. The formation process of the nanoparticles is discussed in terms of the optical decomposition of molecules in the highly intense optical field generated by femtosecond laser irradiation.