Versatile hybrid colloidal spheres, self-assembled through the association of cationic peptide and polyoxometalate clusters, are not only responsive towards external stimuli but also show novel, adaptive inclusion properties. The adaptive nature of hybrid colloidal spheres is utilized to encapsulate a wide variety of guest materials ranging from water-soluble molecules to hydrophobic nanoparticles and hydrophilic inorganic nanoparticles.