Biomimicry and the development of sophisticated materials can derive inspiration from the nanoscale component orientation and hierarchical structures found in living organisms. Herein, a simple and flexible strategy to construct a sophisticated hierarchical structure based on electrophoretic and electrochemical deposition is reported. Cellulose nanofibres (CNFs), which were used as model materials, were deposited on anode in an aqueous dispersion and fixed in an oriented state, which could be seamlessly altered from horizontal to vertical orientation relatively to the electrodes depending on the applied voltage between the electrodes. The oriented CNF hydrogels not only exhibited anisotropic mechanical properties but also formed complex orientations and hierarchical structures, such as cartilage- and plant stem-like configurations upon varying the electrode shape and applied voltage. This electrophoretic and electrochemical approach was also applied to achieve control over the drying-related shrinkage of the CNF hydrogels, which enabled the fabrication of highly functional dried moulded materials made of rigid CNFs. This simple and flexible technology has the potential to be applied to various materials and thus is expected to contribute to a wide range of fields, such as biomimicry, the formation of highly functional materials made of nanomaterials, and the production of sustainable and functional mouldings.