Hydrogen Bond-Driven Hierarchical Assembly of Single-Walled Carbon Nanotubes for Ultrahigh Textile Capacity

Hydrogen-bond-driven 1D assembly of carbon nanotubes dispersed in organic solvents remains challenging owing to difficulties associated with achieving high oxidation levels and uniform dispersion. Here, we introduced a bioinspired wet-spinning method that utilizes highly oxidized single-walled carbon nanotubes dispersed in organic solvents without superacid or dispersants. By incorporating submicrometer-sized graphene oxide nanosheets, we facilitated the ejection of 1.5 wt % spinning dopes, which formed an interconnected network via hydrogen bonding during coagulation. In this process, swollen carbon nanotube fibers from a multihole spinneret were merged into a single filament via interdigitation, similar to the process observed in spider silk spinning. The resulting interdigitated and conducting carbon nanotube fibers with hierarchical structures serve as versatile textile electrodes in applications such as sensitive textile gas sensors and excellent textile supercapacitors, exhibiting a capacitance of 320 F g^-1 at an extremely high current density of 32 A g^-1. We establish a robust platform for textile electronics, highlighting the significant potential of our bioinspired approach.