High content carbon nanotubes mats have been produced to a range of thicknesses and diameters by covalent bonded cross-linking of thiolated multi-walled carbon nanotubes. The Michael addition pathway was used to cross-link benzoquinone to thiol groups attached to the surface of the nanotubes. The mats were characterized by a variety of techniques including X-ray photoelectron spectroscopy, tensile strength as well as qualitative structural analysis by scanning electron microscopy. It was found that the optimum ratio by weight for cross-linking benzoquinone to thiolated carbon nanotubes was ca. 5:1. This work provided a simple route to the production of mats without high pressure processing or irradiation techniques generally used to produce Buckypaper which can require pressure control chambers, argon and hydrogen ion beams and high temperatures. The mat surface can be further functionalized with nanoparticles to form advanced carbon composite materials.