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Nanotubes of carbon and other materials are arguably the most fascinating materials playing an important role in nanotechnology today. Their unique mechanical, electronic, and other properties are expected to result in revolutionary new materials and devices. However, these nanomaterials, produced mostly by synthetic bottom-up methods, are discontinuous objects, and this leads to difficulties with their alignment, assembly, and processing into applications. Partly because of this, and despite considerable effort, a viable carbon nanotube–reinforced supernanocomposite is yet to be demonstrated. Advanced continuous fibers produced a revolution in the field of structural materials and composites in the last few decades as a result of their high strength, stiffness, and continuity, which, in turn, meant processing and alignment that were economically feasible. Fiber mechanical properties are known to substantially improve with a decrease in the fiber diameter. Hence, there is a considerable interest in the development of advanced continuous fibers with nanoscale diameters. However, conventional mechanical fiber spinning techniques cannot produce fibers with diameters smaller than about 2 μm robustly. Most commercial fibers are several times that diameter, owing to the trade-offs between the techno¬logical and economic factors.