Metal nanoparticles show a particularly strong interaction with light, which is the basis for nanoparticle plasmonics. One of the main goals of this emerging research field is the alignment of nanoparticles and their integration into sophisticated nanostructures providing a tailored interaction with light. This assembly of nanoparticles at well-controlled substrate sites often involves expensive technological approaches, such as electron beam lithography in order to fabricate the nanoparticle structures. Furthermore difficult numerical simulations are needed to predict their optical properties. Both requirements, fabrication and prediction, complicate a cost-efficient exploitation of nanoparticle plasmonics in optoelectronic devices. Here we show that silver nanoparticles deposited under exposure to visible light arrange in a way that the resulting structure shows an optimized interaction with that light. This way, the light not only controls the nanoparticle alignment with an estimated accuracy of well below 20 nm during deposition from the liquid phase, but also defines the optical properties of the growing structure, and therefore complicated prediction is not needed.