Epoxy acrylate (EA) composites containing graphite oxide (GO), graphene and nitrogen-double bond functionalized graphite oxide (FGO) were fabricated using UV-radiation and electron beam radiation via in-situ polymerization. Graphene and FGO were homogenously dispersed in EA matrix and enhanced properties, including thermal stability, flame retardancy, electrical conductivity and reduced deleterious gas releasing in thermo decomposition were obtained. Microscale combustion colorimeter results illustrated improved flame retardancy; EA/FGO composites achieved a 29.7% reduction in total heat release (THR) when containing only 0.1% FGO and a 38.6% reduction in peak-heat release rate (PHRR) when containing 3% FGO. The onset decomposition temperatures were delayed and the maximum decomposition values were reduced, according to thermogravimetric analysis which indicated enhanced thermal stabilities. The electrical conductivity was increased by 6 orders of magnitude (3% graphene) and the deleterious gas released during the thermo decomposition was reduced with the addition of all the graphite samples. This study represented a new approach to functionalize GO with flame retardant elements and active curable double bond to achieve better dispersion of GO into polymer matrix to obtain nanocomposites and paved a way for achieving graphene-based materials with high-performance of graphene in enhancement of flame retardancy of polymers for practical applications.