The next generation of thermal interface materials (TIMs) are currently being developed to meet the increasing demands of high-powered semiconductor devices. In particular, a variety of nanostructured materials, such as carbon nanotubes (CNTs), are interesting due to their ability to provide low resistance heat transport from device-to-spreader and compliance between materials with dissimilar coefficients of thermal expansion (CTEs), but few application-ready configurations have been produced and tested. Recently, we have undertaken major efforts to develop functional nanothermal interface materials (nTIMs) based on short, vertically aligned CNTs grown on both sides of a thin interposer foil and interfaced with substrate materials via metallic bonding. A high-precision 1D steady-state test facility has been utilized to measure the performance of nTIM samples, and more importantly, to correlate performance to the controllable parameters. In this paper, we describe our material structures and the myriad permutations of parameters that have been investigated in their design. We report these nTIM thermal performance results, which include a best to-date thermal interface resistance measurement of 3.5 mm2 K/W, independent of applied pressure. This value is significantly better than a variety of commercially available, high-performance thermal pads and greases we tested, and compares favorably with the best results reported for CNT-based materials in an application-representative setting.