Velvet worms eject a fluid capture slime that can be mechanically drawn into stiff biopolymeric fibres. Remarkably, these fibres can be dissolved by extended exposure to water, and new regenerated fibres can be drawn from the dissolved fibre solution-indicating a fully recyclable process. Here, we perform a multiscale structural and compositional investigation of this reversible fabrication process with the velvet worm Euperipatoides rowelli, revealing that biopolymeric fibre assembly is facilitated via mono-disperse lipid-protein nanoglobules. Shear forces cause nanoglobules to self-assemble into nano- and microfibrils, which can be drawn into macroscopic fibres with a protein-enriched core and lipid-rich coating. Fibre dissolution in water leads to re-formation of nanoglobules, suggesting that this dynamic supramolecular assembly of mechanoresponsive protein-building blocks is mediated by reversible non-covalent interactions. These findings offer important mechanistic insights into the role of mechanochemical processes in bio-fibre formation, providing potential avenues for sustainable material fabrication processes.Velvet worms expel a fluid slime that, under shear force, forms stiff fibres that can be dissolved and then regenerated. Here, the authors reveal that the recyclability of these biopolymers relies on mechanoresponsive lipid-protein nanoglobules in the slime that reversibly self-assemble into fibrils.