Epoxy resins find versatile and massive use in such areas as coatings, adhesives, composite materials and electronic packaging, owing to their outstanding properties and favorable processability. However, they still suffer from high flammability. Furthermore, suppressing smoke release from burning of epoxy materials is quite challenging and far away from being well resolved. In this proposal we intent to develop a new generation halogen-free high-performance epoxy nanocomposites characterized by high fire retardant efficiency and low smoke release with satisfactory mechanical, thermal and other properties. First we shall design and prepare several novel graphene oxide/layered double hydroxide (GO/LDH) hybrids as multifunctional reactive fire retardants for epoxy resins, by wisely integrating LDH, GO and organic phosphorus into one component via a more sophisticated and innovative approach. Then these hybrids will be dispersed into an epoxy/hardener matrix at a nanoscale to yield the GO/LDH/epoxy nanocomposites. The curing reaction, reaction kinetics, mechanisms and rheological performance of these nanocomposites will be highlighted based on thermal and rheological analyses to reach a deep insight into how to optimize curing and processing conditions. The fire retardancy, smoke release, and mechanisms of the cured nanocomposites will be studied using cone calorimeter, TGA, UL94 and LOI tests, SEM, XPS, etc. The mechanical, thermal and other properties of the nanocomposites will be systematically examined. Eventually the structure-property relationship of these nanocomposites will be established. Predictedly, these epoxy nanocomposites will have not only much enhanced flame retardancy and lowered smoke release but also satisfactory mechanical, thermal and other properties. Our study will pave a new way of design, preparation and applications of GO/LDH-based high efficient, multifunctional flame retardants in the field of high-performance epoxy nanocomposites.