matrices can show their unique intrinsic features. [5][6][7] Many hybrid composites and devices with excellent performance often require high doping concentration of functional materials. However, high doping ratio tends to result in adverse effects such as dropped transmittance caused by Rayleigh scattering, [8] weakened optoelectronic and mechanical performance. [9,10] Therefore, maintaining the intrinsic properties of nanoparticles while improving the doping concentration of nanomaterials becomes an urgent subject. There are two approaches to limit nanomaterials in substrates: physical dispersion and chemical dispersion. Physical dispersion of guest materials in host matrices is a conventional approach to prepare hybrid composites. Due to the weak physical interaction, the performance usually is impaired. Compared with physical dispersion, the covalent bond can prevent the phase separation existing in hybrid materials. [11] Among these ways, sol-gel method is a helpful technique to modify nanomaterials and prepare nano-or macroscale organic-inorganic hybrid materials such as glasses, ceramics, films, coatings, fibers, and powders. [12] Silane coupling agents or organosilicon polymers (silicone oil, resin, rubber, etc.) are introduced in the route based on the advantages of simultaneously possessing hydrophilic and lipophilic groups. First, they can elevate the dispersibility of nanomaterials in solutions. Second, they successfully link organic and inorganic phases with covalent bonds. Third, the introduction of silicon promotes the radiation recombination of electron/hole pairs through providing different surface states. There are five empty d orbitals of a silicon atom, where can be occupied by electrons of connected atoms or functional groups to form a dπ-pπ bond. [13] Owing to the above features, the hybrid materials inherit the superiorities of organosilanes: excellent resistance against high temperature; [14] stability under UV radiation; [15] lower surface tension, lower surface energy, and more prominent film-forming ability. [13] Since the discovery in 2004, carbon dots (CDs) have become promising issues due to their outstanding optical properties, such as high quantum yield (QY), photobleaching resistance, upconversion photoluminescence (PL). [16][17][18][19][20] In previous works, a concept of one-step prefunctionalization was brought up, using citric acid and long-chain amino-silanes as starting materials to prepare silane-functionalized CDs (SiCDs). [18] These types of CDs represent either "silane-functionalized carbon dots" or Nanomaterials usually manifest unique properties in solutions but will be undermined in the solid state. It is necessary to incorporate them into substrates or hybrid them with other functional materials for multiple devices and applications. Though there are a variety of methods to inherit their intrinsic properties like fluorescent and mechanical performance, most nanohybrid materials would lose their transparency irreversibly when construct solid-state devices. As a hot t...