The first use of an organosilane as a coordinating solvent to synthesize highly luminescent (quantum yield = 47%) amorphous carbon dots (CDs) in one minute is reported. The CDs, which benefit from surface methoxysilyl groups, have a diameter of ~0.9 nm and can easily be fabricated into pure CD fluorescent films or monoliths simply by heating them at 80 ºC for 24 h. Moreover, the non‐water‐stable CDs can be further transformed into water‐soluble CDs/silica particles, which are biocompatible with and nontoxic to the selected cell lines in our preliminary evaluation. The proposed novel synthetic route is believed to provide an alternative synthesis route and should inspire more research into the origin and applications of CDs, as well as delivering CD‐based materials. Bright dots: The first use of an organosilane as a coordinating solvent to synthesize highly luminescent (quantum yield = 47%) amorphous carbon dots (CDs) in one minute is reported. The CDs, which benefit from surface methoxysilyl groups, have a diameter of ≈0.9 nm and can easily be fabricated into fluorescent films or monoliths by heating them at 80 ºC for 24 h. Moreover, the non‐water‐stable CDs can be further transformed into water‐soluble CDs/silica particles, which are biocompatible with and nontoxic to the selected cell lines in our preliminary evaluation.