Summary: | Among the many potential applications of carbon nanotubes (CNT), its usage to strengthen polymers has been paid considerable attention due to the exceptional stiffness, excellent strength, and the low density of CNT. This has provided numerous opportunities for the invention of new material systems for applications requiring high strength and high modulus. Precise control over processing factors, including preserving intact CNT structure, uniform dispersion of CNT within the polymer matrix, effective filler–matrix interfacial interactions, and alignment/orientation of polymer chains/CNT, contribute to the composite fibers’ superior properties. For this reason, fabrication methods play an important role in determining the composite fibers’ microstructure and ultimate mechanical behavior. The current state-of-the-art polymer/CNT high-performance composite fibers, especially in regards to processing–structure–performance, are reviewed in this contribution. Future needs for material by design approaches for processing these nano-composite systems are also discussed.
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