Multi-scale assembly and structure-process-property relationships in nanocellulosic materials

Recently, we have witnessed an unprecedented rapidity in scientific and engineering advances for the controlled structuring of nanocellulose-based materials to target novel functionalities and properties. Various processing methods are used to structure such nanosized materials, providing a wide range of final nano-architectures with a versatile range of morphologies and properties. Yet, the structures of these cellulosic materials and, therefore, their desirable properties are strongly linked to the intrinsic properties − morphology, crystallinity, mechanical, optical and thermal − of nanocellulose. These features are in turn dictated by the origin of the raw materials, methods used to isolate them, and their surface topochemistries. Interdisciplinary knowledge culled from a range of disciplines including engineering, chemistry, physics, and materials science, is therefore necessary to develop and understand the controlled structure of nanocellulose. This review provides a critical in-depth examination of the correlation of source-property-assembly-application relationships for several nanocellulose-based structured materials. It holistically integrates these elements across the entire lifecycle of nanocellulose. By critically comparing how different sources and production techniques influence structured materials, such as fibrous, porous networks or layered composites, it provides nuanced understanding that fills the gaps in the current literature which will advance the field by interlinking these relationships to optimize nanocellulose-based materials for advanced applications.