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