We report the preparation and encapsulation properties of stimuli-responsive nanocapsules, self-assembled by the noncovalent interactions of cyclodextrinappended polymers (host) and complementary ferrocene or azobenzene carriers (guest). The encapsulation process was significantly accelerated by applying (electro) chemical or light stimulus, enabling the easier and faster diffusion of guest molecules through the polymer layers. The nanocapsules were characterized by dynamic light scattering, confocal microscopy, ESEM, AFM, UV–visible and fluorescence spectroscopy, and electrochemical techniques. The encapsulation and release properties of the nanocapsules were reversible and could be repeated several times, indicating that the prepared nanoassemblies are very stable.