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This work describes a simple route for the production of carbon nanotube mats without high pressure processing or irradiation techniques that are generally used to produce Buckypaper. The Michael addition pathway was used to covalently cross-link thiol functionalized multi-walled carbon nanotubes with benzoquinone to produce high content nanotube mats of various thicknesses and diameters. The mats were characterized by a variety of techniques including X-ray photoelectron spectroscopy, tensile strength measurements as well as qualitative structural analysis through scanning electron microscopy. It was found that the weight ratio for optimum cross-linking to be ca. 5:1 (benzoquinone:MWCNT-SH) and that the mat surface can be further functionalized with nanoparticles to form advanced carbon composite materials.