Multi‐walled carbon nanotube (MWNT)‐sheet‐reinforced bismaleimide (BMI) resin nanocomposites with high concentrations (∼60 wt%) of aligned MWNTs are successfully fabricated. Applying simple mechanical stretching and prepregging (pre‐resin impregnation) processes on initially randomly dispersed, commercially available sheets of millimeter‐long MWNTs leads to substantial alignment enhancement, good dispersion, and high packing density of nanotubes in the resultant nanocomposites. The tensile strength and Young's modulus of the nanocomposites reaches 2 088 MPa and 169 GPa, respectively, which are very high experimental results and comparable to the state‐of‐the‐art unidirectional IM7 carbon‐fiber‐reinforced composites for high‐performance structural applications. The nanocomposites demonstrate unprecedentedly high electrical conductivity of 5 500 S cm−1 along the alignment direction. Such unique integration of high mechanical properties and electrical conductance opens the door for developing polymeric composite conductors and eventually structural composites with multifunctionalities. New fracture morphology and failure modes due to self‐assembly and spreading of MWNT bundles are also observed.

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Preformed carbon nanotube thin films (10-20 microm), or buckypapers (BPs), consist of dense and entangled nanotube networks, which demonstrate high electrical conductivity and provide potential lightweight electromagnetic interference (EMI) solutions for composite structures. Nanocomposite laminates consisting of various proportions of single-walled and multi-walled carbon nanotubes, having different conductivity, and with different stacking structures, were studied. Single-layer BP composites showed shielding effectiveness (SE) of 20-60 dB, depending on the BP conductivity within a 2-18 GHz frequency range. The effects on EMI SE performance of composite laminate structures made with BPs of different conductivity values and epoxy or polyethylene insulating layer stacking sequences were studied. The results were also compared against the predictions from a modified EMI SE model. The predicted trends of SE value and frequency dependence were consistent with the experimental results, revealing that adjusting the number of BP layers and appropriate arrangement of the BP conducting layers and insulators can increase the EMI SE from 45 dB to close to 100 dB owing to the utilization of the double-shielding effect.

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