Abstract
Natural fibre composites have been utilised in many applications such as automotive and buildings, thanks to their high specific properties and environmentally friendly nature. However, the incompatibility between hydrophilic natural fibres and hydrophobic polymer resins remains a longstanding issue in natural fibre composites. Inspired by nature 's hierarchical structures and tailored functionalities, a nano-engineered hierarchical natural fibre composite has been developed in this study, utilising cellulose nanocrystals (CNCs) as localised nanoreinforcements at flax surfaces in a flax/bio-epoxy system. A simple and versatile spray coating technique was used to deposit CNCs on unmodified flax fibres, without using any chemical solvents. With the increased surface roughness and hence improved epoxy wetting on nano-engineered flax surfaces (3 wt% CNC loading), mechanical properties of the hierarchical composites have been significantly improved, with a 60 % increase in interlaminar shear strength, indicating an enhanced interfacial load transfer between flax and epoxy, alongside improved flexural modulus (14 %) and strength (23 %). This green approach without using any chemicals provides a scalable and sustainable way to develop tailored interfaces for natural fibre composites with enhanced resin wetting and mechanical properties.