Carbon nanotubes (CNTs) dispersion in aqueous and organic media was studied in presence of poly(N-(2-(dimethylamino) ethyl)-methacrylate) (PDMAEMA). Theoretical and experimental studies were performed in order to emphasize the CNT⋯PDMAEMA character of the interactions. The rationalization of a CH⋯π interaction was fully supported by molecular dynamics simulations and confirmed the potential role of PDMAEMA to behave as anchoring agent toward the CNTs. This efficient strategy was applied to the formation of polylactide-based CNTs nanocomposite materials, targeting biomedical applications.