Citrate-capped gold nanoparticles with narrow diameter distribution were prepared by the reduction of chloroauric acid with borohydride. After the gold nanoparticles were transferred to toluene solution through ligand conformation change, close-packed two-dimensional nanocrystal lattices were obtained on transmission electron microscopy (TEM) copper grids by evaporating approximately 10 μL of concentrated particle dispersion. The formation of the thiolate gold nanoparticles was investigated by UV-visible absorption spectroscopy and FTIR spectra. The 2D Fourier transform power spectra of the monolayer confirmed the supperlattices' hexagonal symmetry. Furthermore, long-range-ordered bilayer superlattices, of which the nanoparticles in the top layer piled on the ones in the bottom layer, could also be observed by transmission electron microscopy.