To facilitate the design of carbon nanotube (CNT)-based hybrid materials, a strategic approach for nanotube dispersion in aqueous media is required. This means that the reactants must exhibit certain selectivity towards both the nanotubes and the solvent medium. The main goal of this study was to prepare new bionanomaterials based on human serum albumin (HSA) and multi-walled CNTs (MWCNTs), under mild conditions and without covalent modification of the nanotubes. Silver nanoparticles (AgNPs) of a controlled particle size, about 2-nm diameter, were prepared and directly deposited onto the HSA-functionalised MWCNTs. The characterisation of AgNP/HSA-MWCNT hybrids prepared was carried out by scanning tunneling microscopy and transmission electron microscopy (TEM). The presence of the AgNPs was corroborated by elemental chemical analysis using TEM-coupled energy-dispersive X-ray spectroscopy. The density of AgNPs coverage is discussed as a function of HSA concentration, the strength of the reducing agent, and the nature of protein employed (HSA vs. bovine serum albumin and rotavirus nucleocapsid protein VP6). (c) 2012 Canadian Society for Chemical Engineering