A method based on the conventional lithographic technique combined with the layer-by-layer (LBL) assembly process is applied to the construction of free-standing micro- and nanostructured matrixes. The method enables controlled shaping and considerable chemical and mechanical stability of the self-assembled monolayers, allowing for high reproducibility in manufacturing. The matrixes are characterized by controlled geometry, surface topography, and chemical composition. The complete architecture is made up of successive layers of intercrossed carbon nanotubes that self-assemble into orderly structures. In particular, the present method aims to create architectures and topographies that mimic those occurring naturally ( native tissue structures). In addition, nanoindentation and nanoscratch techniques were used to evaluate the mechanical properties of the carbon nanotube-based matrixes.