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Carbon nanotubes (CNTs) are ideal scaffolds to design and architect high-perform‐ ance composites at high CNT volume fractions. In these composites, the CNT align‐ ment determines the level of aggregation and the structure morphology, and thus the load transfer efficiency between neighboring CNTs. Here, we discuss two major solutions to produce high-volume fraction CNT composites, namely the layer-bylayer stacking of aligned CNT sheets and the stretching of entangled CNT webs (networks). As inspired by the growth procedure of natural composites, the aggrega‐ tion of CNTs can be well controlled during the assembling process. As a result, the CNTs can be highly packed, aligned, and importantly unaggregated, with the impregnated polymers acting as interfacial adhesion or mortars to build up the composite struc‐ ture. The CNT/bismaleimide composites can yield a super-high tensile strength up to 6.27–6.94 GPa and a modulus up to 315 GPa.

Bio-inspired Design and Fabrication of Super-Strong and Multifunctional Carbon Nanotube Composites