The self-assembly of well-defined polypeptide-based diblock copolymers into micelles and vesicles is presented. The stimuli-responsive behavior of polypeptides to pH and ionic strength is used to produce stimuli-responsive nanoparticles with controlled size and shape. Results focusing on micelles and vesicles obtained from polypeptide-based diblock copolymers that are particularly promising for biomedical applications are detailed by means of static and dynamic light scattering analysis, UV circular dichroism, NMR and small angle neutron scattering experiments. Also systems able to form vesicles with a narrow size distribution at basic and acid pH going through a single molecule intermediate state are presented. These nanoparticles are particularly interesting for encapsulation and delivery purpose at a controlled pH. (c) 2006 Elsevier B.V. All rights reserved.