This work investigates ways to fabricate composite macro-structures made of carbon nanotubes in combination with polymers and metals to enhance membrane lifespan and performance. Carbon nanotube Buckypapers were used as a template to engineer composite structures. The new materials have been thoroughly characterized for their thermal, structural and performance characteristics. The permeation and adsorption of gas and water vapor, as well as the membranes’ performance in desalination by direct contact membrane distillation, were tested and compared with polymeric benchmarks.