Ultra‐High Toughness Fibers Using Controlled Disorder of Assembled Aramid Nanofibers

Abstract Assembling nanoscale building blocks with reduced defects has emerged as a promising approach to exploit nanomaterials in the fabrication of simultaneously strong and tough architectures at larger scales. Aramid nanofibers (ANFs), a type of organic nanobuilding block, have been spotlighted due to their superior mechanical properties and thermal stability. However, no breakthrough research has been conducted on the high mechanical properties of a structure composed of ANFs. Here, assembling ANFs into macroscale fiber using a simultaneous protonation and wet‐spinning process is studied to reduce defects and control disorder. The ANF‐assembled fibers consist of hierarchically aligned nanofibers that behave as a defective law structure, making it possible to reach a Young's modulus of 53.15 ± 8.98 GPa, a tensile strength of 1,353.64 ± 92.98 MPa, and toughness of 128.66 ± 14.13 MJ m⁻³. Compared to commercial aramid fibers, the fibers exhibit ≈1.6 times greater toughness while also providing specific energy to break as 93 J g⁻¹. Furthermore, this shows recyclability of the ANF assembly by retaining ≈94% of the initial mechanical properties. This study demonstrates a facile process to produce high stiffness and strength fibers composed of ANFs that possess significantly greater toughness than commercial synthetic fibers.