Nano-crystalline silicon attracts scientific and technological interest due to its unique tunable optical and electronic properties, which could open up the way to novel applications in fields like photovoltaics, electronics and optoelectronics. Nevertheless, the high processing temperatures and low throughputs of standard synthesis routes hinder many possible technological advances. This work presents a high-throughput technique for room-temperature synthesis of highly crystalline nanoparticle-assembled silicon thin films. Its distinctive feature is the segmentation of the deposition process in two steps: (i) nanoparticle (NP) synthesis in non-thermal plasma, and (ii) ballistic growth of NP-assembled films through a supersonic jet. Nanoparticle-assembled silicon films showing up to 50% of the bulk silicon density are synthesized with crystalline fractions and crystallite sizes in the 0–72% and 2–5.5 nm ranges …