Polypeptide-based diblock copolymers forming either well-defined self-assembled micelles or vesicles after direct dissolution in water or in dichloromethane have been studied combining light and neutron scattering with electron microscopy experiments. The size of these structures could be reversibly manipulated as a function of environmental changes such as pH and ionic strength in water. Compared to other pH-responsive self-assembled systems based on "classical" polyelectrolytes, these polypeptide-based nanostructures present the ability to give a response in highly salted media as the chain conformational ordering can be controlled. This makes these micelles and vesicles suitable for biological applications: they provide significant advantages in the control of the structure and function of supramolecular self-assemblies.