Controlled growth of organic multilayers from periodic gold dot arrays on SiO 2 surfaces has been used to create complex overlayer structures. Nanosphere lithography (NSL) was first used to produce uniform metal patterns with particle sizes of 40 nm, spaced by gaps of 80 nm. These particles served as the nucleation centers for layer-by-layer growth of organic/metal ion complexes. The resulting structures can either be isolated adsorbed dot structures on a continuous surface or continuous networks of the adsorbed materials with isolated arrays of SiO 2 surface dots. Step-by-step organic multilayer growth from small isolated centers enables us to monitor each process step by direct surface imaging techniques. Further metal evaporation and lift-off of the organic layers creates star-shaped gold structures within the original array.