Jae Seo Park

Lightweight structural materials are commonly used as effective fillers for advanced composites with high toughness. This study focused on enhancing the toughness of direct‐spun carbon nanotube yarns (CNTYs) by controlling the micro‐textural structure using a water‐gap‐based direct spinning. Drawing inspiration from the structural features of natural spider silk fibroin, characterized by an α‐helix in the amorphous region and β‐sheet in the crystalline region, multiscale bundles within CNTYs are reorganized into a unique nano‐coil‐like structure. This nano‐coiled structure facilitated the efficient dissipation of external mechanical loads through densification with the rearrangement of multiscale bundles, improving specific strength and strain. The resulting CNTYs exhibited exceptional mechanical properties with toughness reaching 250 J g −1 , making them promising alternatives to commercially available fibers in lightweight, high‐toughness applications. These findings highlight the significance of nano‐coiling engineering for emulating bio‐inspired micro‐textural structures, achieving remarkable enhancement in the toughness of CNTYs.