This research delves into the experimental and theoretical exploration of the mechanical and viscoelastic characteristics of nano-composites consisting of amine-functionalized graphene (AFG) integrated into carbon fiber/epoxy matrices. Through a combination of experimental characterization and theoretical modelling, we examine the synergistic effects arising from the incorporation of AFG on the mechanical behavior of the nanocomposites. Mechanical tests encompassing tensile, compressive, and flexural evaluations unveil notable enhancements in stiffness, strength, and fracture toughness when compared to conventional carbon fiber/epoxy systems Young’s modulus and tensile strength values for 1AFG/CFEC can be increased by a maximum of 60.1% and 59.3% compared to EpC, respectively. Concurrently, dynamic mechanical analysis (DMA) is utilized to elucidate the viscoelastic response of the nanocomposites across a spectrum of temperatures and frequencies. Theoretical investigations, employing finite element analysis (FEA) and molecular dynamics simulations, offer insights into the underlying mechanisms governing the observed mechanical and viscoelastic properties. Also, for 1AFG/CFEC nanocomposite, the glass transition temperature (Tg) can be expanded by 65.2% contrasted with the epoxy composite (EpC).