We demonstrate a method for synthesizing free standing silicon nanocrystals in an argon/silane gas mixture by using a remote expanding thermal plasma. Transmission electron microscopy and Raman spectroscopy measurements reveal that the distribution has a bimodal shape consisting of two distinct groups of small and large silicon nanocrystals with sizes in the range 2–10 nm and 50–120 nm, respectively. We also observe that both size distributions are lognormal which is linked with the growth time and transport of nanocrystals in the plasma. Average size control is achieved by tuning the silane flow injected into the vessel. Analyses on morphological features show that nanocrystals are monocrystalline and spherically shaped. These results imply that formation of silicon nanocrystals is based on nucleation, i.e., these large nanocrystals are not the result of coalescence of small nanocrystals. Photoluminescence measurements show that silicon nanocrystals exhibit a broad emission in the visible region peaked at 725 nm. Nanocrystals are produced with ultrahigh throughput of about 100 mg/min and have state of the art properties, such as controlled size distribution, easy handling, and room temperature visible photoluminescence.