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The continuous flow assembly of colloidal nanoparticles from aqueous suspensions into macroscopic materials in a field-assisted double flow focusing system offers an attractive way to bridge the outstanding nanoscale characteristics of renewable cellulose nanofibrils (CNFs) at scales most common to human technologies. By incorporating single-walled carbon nanotubes (SWNTs) during the fabrication process, high-performance functional filament nanocomposites were produced. CNFs and SWNTs were first dispersed in water without any external surfactants or binding agents, and the resulting nanocolloids were aligned by means of an alternating electric field combined with extensional sheath flows. The nanoscale orientational anisotropy was then locked by a liquid−gel transition during the materials assembly into macroscopic filaments, which greatly improved their mechanical, electrical, and liquid sensing properties. Significantly, these findings pave the way toward the environmentally friendly and scalable manufacturing of a variety of multifunctional fibers for diverse applications.