Carbon nanotubes (CNTs) have received extensive attention due to their extraordinary properties in electronic conduction, [ 1 ] heat transfer, [ 2 ] and mechanical strength. [ 3 ] Materials with unparallel performance, such as super-strong, lightweight e-textiles, can be fabricated from CNTs, suggesting a future revolution in materials science. Thus, the emerging CNT technology will largely depend on the development of effective spinning and post-spinning processes to realize such unprecedented materials. Two widely implemented strategies for fabricating CNT fi bers are in-solution [4][5][6][7] and solid-state spinning techniques. The in-solution spinning of CNTs can produce continuous CNT fi bers; however, homogeneous dispersion of CNTs in the solvent is necessary for proper spinning. Moreover, the properties of the CNT fi bers strongly depend on the methods of CNT dispersion. An alternative strategy is solid-state spinning, [8][9][10][11][12][13][14][15][16][17] which allows avoidance of CNT dispersion in solvents and for various post-spinning processes to be applied with ease. Twisting, [10][11][12][13][14][15][16] densifi cation, [ 9 , 18 ] and infi ltration [ 8 , 19,20 ] are examples of post-spinning processes, and the main purpose of the spinning and post-spinning processes is to enhance the mechanical properties of CNT fi bers. Despite the effort that has been made, however, fabrication of strong CNT fi bers remains a great challenge.The strong protein-based adhesives found in marine mussel Mytilus edulis , provide an important insight into the development of post-spinning processes of CNT fi bers. The mussel secretes special adhesive foot proteins that undergo rapid solidifi cation in seawater. At a molecular level, the unusual amino acid 3,4-dihydroxy-L -phenylalanine (DOPA) found in the adhesive proteins functions as a molecule that is responsible for the solidifi cation by oxidative chemical crosslinking. [21][22][23][24] From a chemical point of view, covalent crosslinking with amines and/or catechol (a side chain of DOPA) or metal coordination are the reactions involved with DOPA, and the reactions are responsible for mechanical reinforcement of the adhesive materials of mussels. [ 25 ] Here, inspired by the molecular mechanics of mussel adhesive formation, we demonstrate a new postspinning process for the fabrication of CNT fi bers ( Figure 1 a,b). By infi ltration of mussel-mimetic adhesive polymers and curing through thermal and metal oxidation, we demonstrate an increase in the tensile strength of CNT fi bers by up to 470%. The study described suggests a general post-spinning approach for enhancement of the mechanical properties of CNT fi bers prepared by various spinning techniques.Vertically well-aligned CNT arrays were grown on Fe-catalystimmobilized (1.7-nm-thick) silicon substrates by plasmaenhanced chemical vapor deposition. Methane (CH 4 ) was used as the carbon source to synthesize CNTs, with argon (Ar), hydrogen (H 2 ), and oxygen (O 2 ) carrier gases. In the presence of Ar gas fl ow...