We summarize our research studies on the synthesis of silicon and germanium nanocrystals and their application to the growth of a variety of thin films, spanning the range from fully disordered amorphous up to fully ordered crystalline. All these films are deposited in a standard radio-frequency glow discharge system at low temperature (~200 °C). We show how the plasma synthesis of silicon nanocrystals, initially a side effect of powder formation, has become over the years an exciting field of research which has opened the way to new opportunities in the field of materials deposition and their application to optoelectronic devices. Our results suggest that epitaxy requires the melting/amorphization of the nanocrystals upon impact on the substrate, the subsequent epitaxial growth being favored on (100) c-Si substrates. As a consequence, the control of the impact energy is a critical aspect of the growth which will require new strategies such as the use of tailored voltage waveforms.