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The new devices and missions to achieve the aims of NASA's Science Mission Directorate (SMD) are creating increasingly demanding thermal environments and applications. In particular, the low conductance of metal-to-metal interfaces used in the thermal switches lengthen the cool-down phase and resource usage for spacecraft instruments. During this work, we developed and tested a vacuum-compatible, durable, heat-conduction interface that employs carbon nanotube (CNT) arrays directly anchored on the mating metal surfaces via microwave plasma-enhanced, chemical vapor deposition (PECVD). We demonstrated that CNT-based thermal interface materials have the potential to exceed the performance of currently available options for thermal switches and other applications.