Arrays of noble metal nanoparticles show potential applications in (bio-)sensing, optical storage, surface-enhanced spectroscopy, and waveguides. For all such potential devices, controlling the size, morphology, and interparticle spacing of the nanoparticles is very important. Here, we combine seed-mediated growth with nanosphere lithography to study the controllable growth of gold nanoparticles (Au NPs), in which the self-assembly monolayer of polystyrene (PS)on a silicon surface is used to guide the modification of alkanesilanes and the subsequent adsorption of gold seeds;seed-mediated growth is applied to controlling the morphology and size of Au NPs. The size of adsorption region (determining the number of adsorbed gold seeds) is controlled by etching PS microspheres with oxygen plasma or annealing PS microspheres at the glass transition temperature. The size and morphology of the Au NPs are controlled by changing growth conditions. In such a way, we have achieved the dual control of the obtained Au NPs. Preliminary results show that this strategy holds a great promise. This approach can also be extended to a wide range of materials and substrates.