Simulation of molecular dynamics (MD) allows mimicking the systematic variation of mechanical properties beyond the capacity of experimental methods. In this review, the status of the molecular modelling, simulation and mechanical and thermal characterisation of graphene and the properties of bulk nanocomposites using MD are extensively examined. The molecular models of graphene (pristine and functionalised), and the most common epoxy matrix with preeminent MD energy minimisation tools are thoroughly examined. The presence of MD’s simulation setup and the computational procedure for different styles of mixing the polymer matrix with graphene as nanofiller are exhaustively reviewed. In particular, in the analysis of several papers on graphene and their composites, it has been noticed that mechanical, thermal and interfacial properties are ubiquitous to most of the engineering applications. In this review, advances in the molecular modelling and simulation of graphene and their composites has been discussed in detail keeping graphene structures, aspect ratio, weight fraction and density effect as major factors. Finally, the research gaps and future scope are discussed, which indeed helps the researchers in scaling up their researches in graphene and their composites, which may further lead to their experimental findings.

Molecular Dynamics (MD) simulations were carried out to investigate the effect of functionalization of graphene on glass transition temperature (T_g) of epoxy composites were built using LY556 epoxy resin cross-linked with DETDA. Three different formats of graphene including pristine, with amine (−NH₂) groups and carboxyl (−COOH) groups respectively involved in the investigation. The simulation results indicated that T_g of the graphene epoxy composites are higher than that of pure epoxy. Furthermore, T_g of composites randomly embedded with functionalized graphene were lower than that with pristine graphene, and T_g of the composites embedded with COOH-graphene was much lower than that with NH₂-graphene. The simulation results of T_g were in good agreement with experimental results indicating that this computational method can be used to predict effectively the T_g of graphene epoxy composites.