Confinement of silicon nanoparticles in silicon nitride instead of an oxide matrix might materially facilitate its potential applications as a light-emitting component in optoelectronics. We report in this letter the production of high-density (up to 4.0×1012/cm2 from micrographs) silicon nanoparticles in SiNx thin films by chemical vapor deposition on cold substrates. Strong room-temperature photoluminescence was observed in the whole visible light range from the deposits that were postannealed at 500 °C for 2 min. The Si-in-SiNx films provide a significantly more effective photoluminescence than Si-in-SiOx fabricated with similar processing parameters: for blue light, the external quantum efficiency is over three times as large. The present results demonstrate that the nanostructured Si-in-SiNx system can be a very competitive candidate for the development of tunable high-efficiency light-emitting devices.