One-Pot Hierarchical Structuring of Nanocellulose by Electrophoretic Deposition

[Image: see text] The orientation control and the formation of hierarchical structures of nanoscale components, such as bionanofibers and nanosheets, have attracted considerable research interest with the aim of achieving sophisticated functional materials. Herein, we report a simple and flexible strategy for constructing sophisticated hierarchical structures through electrophoretic and electrochemical deposition. Cellulose nanofibers (CNFs), which are used as model materials, are deposited on an anode in an aqueous dispersion and seamlessly oriented from horizontal to vertical relatively to the electrode by adjusting the applied voltage between the electrodes. The oriented CNF hydrogels not only exhibit anisotropic mechanical properties but also form complex orientations and hierarchical structures, such as cartilage- and plant stem-like configurations in response to electrode shape and applied voltage. This simple and flexible technique is expected to be applicable to various materials and contribute to a wide range of fields that include biomimicry, functional nanomaterials, and sustainable and functional moldings.