Silicon-based thin-films and nanostructures are of paramount importance in a wide range of applications, including microelectronics, photovoltaics, large area sensors, as well as biomedicine. The wide accessibility of silicon and its relatively low cost have driven a continuous improvement of the technology based on this element. Plasma technology has been widely used for the synthesis of coatings and nanostructures based on silicon. Moreover, it has given a fundamental contribution for continuously improving the control of the physicochemical properties of silicon-based materials, and for allowing the synthesis of nanometric structures with well-defined shape and morphology. In this work, we have reviewed the most interesting developments of plasma-assisted processed for the synthesis of Si-based materials, both inorganic and organic, in the last five years. A special attention has been given to the new techniques, or modifications of already existing ones, that open new possibilities for the synthesis of materials with new properties, as well as nanostructures with novel characteristics.