Mimicking Nature implies the use of bio-inspired hierarchical designs to manufacture nanostructured materials. Such materials should be produced from sustainable sources (e.g., biomass) and through simple processes that use mild conditions, enabling sustainable solutions. The combination of different types of nanomaterials and the implementation of different features at different length scales can provide synthetic hierarchical nanostructures that mimic natural materials, outperforming the properties of their constitutive building blocks. Taking recent developments in flow-assisted assembly of nanocellulose crystals as a starting point, we review the state of the art and provide future perspectives on the manufacture of hierarchical nanostructured materials from sustainable sources, assembly techniques, and potential applications.