The use of organosilanes as surface functionalising materials has been investigated as a precursor to the adsorption of ligand stabilised gold natioparticles and the build-up of nanoparticle/polymer multilayer films. The purpose of surface functionalisation here is to produce a uniform surface with the maximum positive charge possible to enable the efficient adsorption of negatively charged gold nanoparticles. It is generally acknowledged that the characteristics of the first layer are important in determining the quality of the subsequent multilayer film and hence careful attention has been paid to its optimisation. Three arninosilanes have been investigated together with various methods for their deposition. The degree of nanoparticle adsorption in the resulting films was characterised using atomic force microscopy and X-ray photoelectron spectroscopy. The surface potential of the aminosilane films was also measured to provide information regarding the surface charge density. Our results show a strong correlation between the nanoparticle density and the initial surface charge density. Films of 3-aminopropyltriethoxysilane adsorbed from toluene yielded the highest level of nanoparticle adsorption.