Dispersibility and interfacial interactions are the important factors to exploit the high potential of nanocarbons for polymer/nanocarbon nanocomposites. However, carbon backbone with low reactivity has often cause agglomerations and defects from the interfaces. The use of surfactants and the surface modifications of nanocarbons have widely been conducted to improve these issues. This paper reviews recent advances in the design of polymer/nanocarbon nanocomposites, focusing on our research on the reinforcement effect of nanodiamond on polymer nanocomposites.