High performance nanocomposites require well dispersion and high alignment of
the nanometer-sized components, at a high mass or volume fraction as well.
However, the road towards such composite structure is severely hindered due to
the easy aggregation of these nanometer-sized components. Here we demonstrate a
big step to approach the ideal composite structure for carbon nanotube (CNT)
where all the CNTs were highly packed, aligned, and unaggregated, with the
impregnated polymers acting as interfacial adhesions and mortars to build up
the composite structure. The strategy was based on a bio-inspired aggregation
control to limit the CNT aggregation to be sub 20--50 nm, a dimension
determined by the CNT growth. After being stretched with full structural
relaxation in a multi-step way, the CNT/polymer (bismaleimide) composite
yielded super-high tensile strengths up to 6.27--6.94 GPa, more than 100%
higher than those of carbon fiber/epoxy composites, and toughnesses up to
117--192 MPa. We anticipate that the present study can be generalized for
developing multifunctional and smart nanocomposites where all the surfaces of
nanometer-sized components can take part in shear transfer of mechanical,
thermal, and electrical signals