The
prospect of developing multifunctional flexible three-dimensional
(3D) architectures based on integrative chemistry for lightweight,
foldable, yet robust, electronic components that can turn the many
promises of graphene-based devices into reality is an exciting direction
that has yet to be explored. Herein, inspired by nature, we demonstrate
that through a simple, yet novel solvophobic self-assembly processing
approach, nacre-mimicking, layer-by-layer grown, hybrid composite
materials (consisting of graphene oxide, carbon nanotubes, and conducting
polymers) can be made that can incorporate many of the exciting attributes
of graphene into real world materials. The as-produced, self-assembled
3D multifunctional architectures were found to be flexible, yet mechanically
robust and tough (Young’s modulus in excess of 26.1 GPa, tensile
strength of around 252 MPa, and toughness of 7.3 MJ m<sup>–3</sup>), and exhibited high native electrical conductivity (38700 S m<sup>–1</sup>) and unrivalled volumetric capacitance values (761
F cm<sup>–3</sup>) with excellent cyclability and rate performance