Because of the strong light absorption and/or scattering, nano scaled gold has many favorable optic and electric properties. With the continuous miniaturization of nano photoelectronic devices and nano electromechanical systems, there is an urgent demand for controllable and tailored gold nanoparticles film with excellent performance. Here, a modified HAuCl4-NaOH-CTAB (cetyltrimethylammonium bromide) aqueous solution system was utilized to self-assembly synthesize gold nanofilm on glass substrates. The high concentration NaOH is not only reducing Au3+ to Au0, but facilitating interfacial assembly of gold nanostructure at liquid–solid interface via etching glass surface. Based on this growth kinetic, the gradient, well-designed and in-situ growing gold nanoparticles film can be achieved on any SiO2 contained substrates by controlling the growth time in the reaction system. Furthermore, the in-situ self-assembled gold nanoparticles film can be act as plasmon substrates for surface-enhanced Raman scattering (SERS) or plasmonic enhanced semiconductor lasing, even gold electrodes.