The CNT sheet fabricated by the floating catalyst chemical vapor deposition (CVD) method has attracted great attention due to its easy fabrication process and promising mass production at low cost. However, the randomly oriented CNT sheet with a loose stacking density shows relatively poor mechanical properties. In this work, a highly aligned dense CNT sheet was successfully fabricated by a simple process of two-time stretching and pressing of a multilayered CVD-grown CNT sheet. Drastic nanotube rearrangements occurred during stretching and pressing processes. A polymer-like tensile necking behavior was observed during the stretching process, accompanied by inter-tube junction breakage due to long-distance slippage. Simultaneously the CNT sheet was thickened after the stretching process due to the increase of the inter-layer space, which could be effectively eliminated by the following pressing treatment. After two-time stretching and pressing, a highly aligned dense CNT sheet was fabricated with the volume density increasing to 0.98 g cm⁻³ (by 109%) and the tensile strength increasing to 598 MPa (by 221%) compared to the as-prepared CNT sheet.

Hierarchical CNT composite yarn muscles with excellent contraction and stability as well as high actuation force were fabricated.

Carbon nanotubes are ideal scaffolds for designing and architecting flexible graphite films with tunable mechanical, electrical and thermal properties. Herein, we demonstrate that the assembly of aligned carbon nanotubes with different aggregation density and morphology leads to different mechanical properties and anisotropic electrical conduction along the films. Using drying evaporation under tension treatment, the carbon nanotubes can be assembled into strong films with tensile strength and Young's modulus as high as 3.2 GPa and 124 GPa, respectively, leading to a remarkable toughness of 54.38 J g⁻¹, greatly outperforming conventional graphite films, spider webs and even Kevlar fiber films. Different types of solvents may result in the assembly of CNTs with different aggregation morphology and therefore different modulus. In addition, we reveal that the high density assembly of aligned CNTs correlates with better electric conduction along the axial direction, enabling these flexible graphite films to be both strong and conductive.