Highly luminescent glass films incorporating hydrophobic quantum dots (QDs) were prepared by a facile layer-by-layer self-assembly method. The surface silanization of hydrophobic CdSe QDs was an important step in the preparation of the thin films. Si lane coupling agents are used as a linker between QD layers. The fabricated glass thin film had good luminescent efficiency of 37%, identical to that of QDs after silanization. The QDs in the thin films were not aggregated, but were in close-packed form and showed good stability.