[[abstract]]We have obtained nanometer sized silicon remnants sequestered in glass matrices by terminating the reaction of pure silicon powders dispersed in the viscous melt at a temperature of 1400 °C. Repeated use of this truncated melt‐particle reaction process dilutes the amount and size of silicon remnants, and bulk samples containing nanosize silicon crystallites embedded in a glass matrix were eventually obtained. These quantum dot sized silicon‐in‐glass materials emit greenish luminescence with peak wavelengths from ≊480 to 530 nm, considerably shorter than the reddish luminescence (at about 700–850 nm) observed in porous silicon structures prepared by electrochemical etching techniques; upon complete digestion of Si particles by th...