Bottom-Up Fabrication was a dreamed of approach in the area of fabrication engineering. The self-assembly of nano-structure is the goal and starts with the self-assembly of nanoparticles under controlled conditions. There was another finding that the size of the self-assembled gold nanoparticles could be controlled with the mole ratio between AuCl4- and thiol. This study showed that the size distribution is controlled via the mole ratio, between AuCl4- and thiol, was proved to be feasible by the experiments. Six different molar ratios of Au/S used in the reactions included 0.25:1, 0.5:1, 1:1, 3:1, 5:1, 8:1, respectively. The size distributions of the gold nanoparticles were measured by Mac-View analysis software and were under a narrow range for each specific molar ratios. High-resolution transmission electron microscope (HR-TEM) was used to derive images of gold nanoparticles, and the range of size in 2~5 nm. The higher the mole ratio between AuCl4- and thiol, the larger the self-assembled gold nanoparticles. The obtained nanoparticle networks could be used in surface nanofabrication, leading to the fabrication of ordered arrays of metal quantum dots.