A process enabling both the controlled growth and positioning of metal nanoparticles (NPs) is reported. Using scanning probe microscopy (SPM) techniques, metal NPs are directly grown in the region of interest via the reduction of metallic ions in a polymer matrix induced by a properly biased SPM tip. The metallic nature of these NPs is established via X-ray diffraction and surface-enhanced Raman spectroscopy experiments. Some initial applications of this process, such as the decoration of carbon nanotubes with metal NPs, are also briefly demonstrated and discussed.