This project develops a systematic and comprehensive understanding of how the mechanical properties of three-dimensional carbon nanotube aerogels depend on pore geometry, pore size distribution, and the characteristics of the junctions between nanotubes to improve the performance and to predict an optimal design of nanotube based porous structures. This project will begin with the development of three-dimensional mechanical models for nanotube aerogels that include realistic network structures as well as nanotube and junction properties that approximate experimental system. The mechanical properties of the aerogels, including modulus and hysteresis, as a function of network and junction parameters will then be measured. By varying the junction properties, the range of available nanotube aerogel properties will be surveyed in order to provide insight and guidance on desirable (and unfavorable) junction characteristics. The guidance from simulations will then be translated to fabricate three-dimensional nanotube networks with diverse junctions that are coated with graphene, covalently crosslinked, and fused with continuous hybridized bonds. The ability to predict, design, and synthesize these structures with computation coupled with experiment will advance the pace at which electrode materials can be designed, and will serve as a model for advancing other porous materials.