To create hierarchically structured nanocomposites in which each sub-layer contributes a distinct function to yield a mechanically integrated macro-scale material is a big challenge nowadays.Nature provides us many fantastic examples, but it is almost beyond our current knowledge how to artificially assemble those nanoscale clusters into large scale materials by the means of biomimetics.Herein, we report some of our recent attempts on the production and investigation of hierarchically structured nanocomposites based on some macroscale architectures of nanoscale carbon materials, e.g.carbon nanotubes (CNTs) and graphenes.