Strong Silkworm Silk Fibers through CNT‐Feeding and Forced Reeling

High-performance silk fibers, with their eco-friendly degradability and renewability, have long captivated researchers as an alternative to synthetic fibers. Spider dragline silk, renowned for its exceptional strength (>1 GPa), has an extremely low yield, hindering its widespread use. While domesticated silkworms (Bombyx mori) can produce silk fibers industrially, their moderate strength (≈0.5 GPa) pales in comparison to the formidable spider dragline silk. In this study, naturally produced strong silkworm silk fibers are reported with a tensile strength of ≈1.2 GPa achieved through combining feeding carbon nanotubes (CNTs) to silkworms and in situ forced reeling for alignment. Molecular dynamics simulations confirm the interaction between the CNTs and silk fibroin, while the forced reeling process aligns these reinforcing fillers and the silk fibroin β-sheet nanocrystals along the fiber axis. Structural analysis reveals a significant enhancement in the content and alignment of β-sheet nanocrystals within the silk fibers, accounting for their superior mechanical properties, including tensile strength of ≈1.2 GPa and Young's modulus of 24.4 GPa, surpassing various types of silkworm silk and spider silk. This advancement addresses the historical trade-off between the strength and scalability of silk, potentially paving the way for eco-friendly, biodegradable, and renewable alternatives to synthetic fibers in a variety of applications.