In this work, the expanding thermal plasma chemical vapor deposition in combination with radio frequency magnetron sputtering is used to deposit dielectric/metal multi-layers with controlled size and density of nanoparticles. The multi-layer structure serves the purpose of increasing the nanoparticle number density, without changing the metal particle size, shape and the interparticle distance. The possibility of independently tuning and, therefore, controlling the nanoparticle size and number density allows developing surface plasmon resonance-based deep-colored coatings. The influence of the number of layers, metal surface area coverage, and thickness of the dielectric layer on the multi-layer nanostructure and on the developed color is presented here in detail. The nanoparticle size and distribution have been measured by transmission electron microscopy. Rutherford back-scattering and infra-red transmission spectroscopy have been used to determine the metal surface coverage and the film chemistry, respectively. Optical properties of the nano-composite layers have been investigated by UV-VIS spectroscopy and exhibit an increase in amplitude of the plasmon absorption spectra at a fixed plasmon resonance frequency with an increase in the number of layers.