Reliably routing heat to and from conversion materials is a daunting challenge for a variety of innovative energy technologies--from thermal solar to automotive waste heat recovery systems--whose efficiencies degrade due to massive thermomechanical stresses at interfaces. This problem may soon be addressed by adhesives based on vertically aligned carbon nanotubes, which promise the revolutionary combination of high through-plane thermal conductivity and vanishing in-plane mechanical stiffness. Here, we report the data for the in-plane modulus of aligned single-walled carbon nanotube films using a microfabricated resonator method. Molecular simulations and electron microscopy identify the nanoscale mechanisms responsible for this property. The zipping and unzipping of adjacent nanotubes and the degree of alignment and entanglement are shown to govern the spatially varying local modulus, thereby providing the route to engineered materials with outstanding combinations of mechanical and thermal properties.nanostructured materials | van der Waals | thermal interface materials | thermoelectrics | energy conversion N anostructured materials provide unique combinations of properties that promise performance breakthroughs for applications ranging from energy conversion to data storage and computation (1-4). In many cases it is the very unusual combination of two properties (2), neither of which is an extreme value when considered alone, that leads to adoption and major performance benefits. An example is the search for a mechanically compliant thermal conductor that can, for example, link semiconducting materials with the metals used for heat spreading and exchange. A particularly compelling case is thermoelectric waste heat recovery systems (3), for which the interfaces between the thermoelectric materials, electrodes, insulators, and heat exchangers must accommodate enormous, repetitive thermomechanical stress. However, nature does not provide a material combining the necessary high thermal conductivity with the required low elastic modulus (5, 6).Vertically aligned carbon nanotube (CNT) films may combine mechanical compliance with high thermal conductivity (7-18), but there have been few reports of the in-plane modulus of these films and little physical explanation for the wide range for the data (2-300 MPa) (19-25). Our previous data for the thickness-dependent in-plane modulus of multiwalled CNT films indicated a strong dependence on the nanotube density and alignment (21), which are linked to the detailed growth details (26-28). Other approaches, such as mesoscopic simulations or atomistic models, found that CNT networks exhibit unique self-organization, including bending and bundling (29-31). Therefore, relating the nanoscale morphological details to the mechanical properties is critical.Combined experimental, theoretical, and computational techniques applied to the more complex and fundamentally challenging single-walled CNT system are presented in this paper, along with the in-plane data for the modulus for sin...