AbstractCarbon nanotube macro-films are two-dimensional films with micrometer thickness and centimeter by centimeter in-plane dimension. These carbon nanotube macroscopic assemblies have attracted significant attention from the material and mechanics communities recently because they can be easily handled and tailored to meet specific engineering needs. This paper reports the experimental methods on the preparation and characterization of single-walled carbon nanotube macro-films, and a statistical mechanics model on the deformation behavior of this material. This model provides a capability to optimize the synthesis process by comparing with the experiments