In this paper, we study the crosslinking route and interface interactions for achieving superior properties in carbon nanotube (CNT)-reinforced epoxy based nanocomposites by using multiscale modelling. For that purpose, polymeric epoxy matrices consisting of EPON 862 epoxy and 15 TETA hardener molecules were coarse-grained and simulated using the dissipative particle dynamics (DPD) method. Furthermore, CNTs were coarse-grained as rigid rods and embedded into the uncrosslinked mesoscopic polymer system. Reverse-mapping of the atomistic details onto coarse-grained models was carried out to allow further simulations at the atomistic scale using molecular dynamics (MD) by keeping the periodicity of the CNTs structure. The 20 mechanism of crosslinking is simulated, and both neat and CNTs-reinforced thermoset nanocomposites with different degrees of crosslinking were reconstructed. Normal stresses in tensile and compressive loading direction up to 0.2% strain were calculated and yield strength (0.2% offset) and compressive/elastic modulus in both normal directions were reported, which match the experimental values as well. Overall, this paper explores a fast and straightforward 25 procedure to bridge periodic mesoscopic structures such as CNTs and their nanocomposites to experimentally tested material properties.