High-density silicon nanoparticles with well-controlled sizes were grown onto cold substrates in amorphous SiNx and SiC matrices by plasma-enhanced chemical vapor deposition. Strong, tunable photoluminescence across the whole visible light range has been measured at room temperature from such samples without invoking any post-treatment, and the spectral features can find a qualitative explanation in the framework of quantum confinement effect. Moreover, the decay time was for the first time brought down to within one nanosecond. These excellent features make the silicon nanostructures discussed here very promising candidates for light-emitting units in photonic and optoelectronic applications.