AbstractAdvanced optical applications of fluorescent carbon dots (C-dots) require highly integrated host-guest solid-state materials with a careful design of C-dots – matrix interface to control the optical response. We have developed a new synthesis based on the grafting of an organo-functional silane (3-glycidyloxypropyltrimethoxysilane, GPTMS) on amino-functionalized C-dots, which enables the fabrication of highly fluorescent organosilica-based hybrid organic-inorganic films through sol-gel process. The GPTMS grafting onto C-dots has been achieved via an epoxy–amine reaction under controlled conditions. Besides providing an efficient strategy to embed C-dots into a hybrid solid-state material, the modification of C-dots surface by GPTMS allows tuning their photoluminescence properties and gives rise to an additional, intense emission around 490 nm. Photoluminescence spectra reveal an interaction between C-dots surface and the polymeric chains which are locally formed by GPTMS polymerization. The present method is a step forward to the development of a surface modification technology aimed at controlling C-dots host-guest systems at the nanoscale.