A practically simple top-down process for the exfoliation of graphene (GN) and few-layer graphene (FLG) from graphite is described. We have discovered that a biocompatible amphiphilic pyrene-based hexahistidine peptide is able to exfoliate, functionalize, and dissolve few layer graphene flakes in pure water under exceptionally mild, sustainable and virtually innocuous low intensity cavitation conditions. Large area functionalized graphene flakes with the hexahistidine oligopeptide (His₆-TagGN = His₆@GN) have been produced efficiently at room temperature and characterized by TEM, Raman, and UV spectroscopy. Conductivity experiments carried out on His₆-TagGN samples revealed superior electric performances as compared to reduced graphene oxide (rGO) and non-functionalized graphene, demonstrating the non-invasive features of our non-covalent functionalization process. We postulated a rational exfoliation mechanism based on the intercalation of the peptide amphiphile under cavitational chemistry. We also demonstrated the ability of His6-TagGN nanoassemblies to self-assemble spontaneously with inorganic iron oxide nanoparticles generating magnetic two-dimensional (2D) His₆-TagGN/Fe₃O₄ nanocomposites under mild and non-hydrothermal conditions. The set of original experiments described here open novel perspectives in the facile production of water dispersible high quality GN and FLG sheets that will improve and facilitate the interfacing, processing and manipulation of graphene for promising applications in catalysis, nanocomposite construction, integrated nanoelectronic devices and bionanotechnology.