Crystalline silicon (Si) is widely used in modern electronics. Si is commonly produced through a series of energy-intensive reactions (>700 째C). It is thus urgent and significant to explore more economically and environmentally-benign synthetic strategies for crystalline Si at low temperature. In this contribution, we report an efficient method to prepare crystalline Si from silicon tetrachloride at the low temperature of 100 째C with an ionic liquid (IL) as electrolyte. Physicochemical characterization revealed that as-deposited crystalline Si with a diamond cubic crystal structure exhibited a dominant (111)-orientation. Moreover, in-depth insights into the growth mechanism of crystalline Si was shed light upon herein. Furthermore, the smart electrodepositing platform of crystalline Si from ILs would open up a new avenue for low-temperature metallurgy of Si.