The continuous production of macroscale filaments of 17 μm in diameter comprising aligned TEMPO-oxidized cellulose nanofibrils (CNFs) is conducted using a field-assisted flow-focusing process. The effect of an AC external field on the material's structure becomes significant at a certain voltage, beyond which augmentations of the CNF orientation factor up to 16% are obtained. Results indicate that the electric field significantly contributes to improve the CNF ordering in the bulk, while the CNF alignment on the filament surface is only slightly affected by the applied voltage. X-ray diffraction shows that CNFs are densely packed anisotropically in the plane parallel to the filament axis without any preferential out of plane orientation. The improved nanoscale ordering combined with the tight CNF packing yields impressive enhancements in mechanical properties, with stiffness up to 25 GPa and more than 63% (up to 260 MPa), 46% (up to 2.8%), and 120% (up to 4.7 kJ/m3) increase in tensile strength, strain-to-failure, and toughness, respectively. This study demonstrates for the first time the control over the structural ordering of anisotropic nanoparticles in a dynamic system using an electric field, which can have important implications for the development of sustainable alternatives to synthetic textiles.
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