will lead to important applications for power generation and more efficient energy utilization, and could play a vital role in meeting our current global energy challenges. [1-5] The potential of a thermoelectric material is typically assessed using the dimensionless figure-of-merit, ZT = α 2 σT/k, where α is the Seebeck coefficient, σ is the electrical conductivity, k is the thermal conductivity, and T is temperature. ZT determines the overall efficiency of thermoelectric energy generation or cooling (via the Onsager reciprocal Peltier effect where current driven through the material generates a thermal gradient) with larger values of ZT resulting in better thermoelectric devices. Current thermoelectric devices are based on materials with ZT ≈ 1. If this value could be increased to 3-4, the resulting gains in the efficiency will allow broad application of thermoelectric devices for energy generation and refrigeration, [6] though low-cost, flexible materials could see important use in mobile and wearable device applications even at much lower ZT. [7-10] Regardless of the targeted application, the materials properties in ZT are usually determined by the same physics and difficult to separately optimize. Carbon nanomaterials have dramatic and often tunable thermal and electronic properties. [11-13] These range from some of the highest known thermal conductivities observed for individual single-walled carbon nanotubes (CNT), [14-18] or suspended single-layer graphene [19] to the recently observed unconventional superconducting phase of bilayer magic-angle twisted graphene. [20] Despite k reaching in excess of 3000 W m −1 K −1 in single nanostructures, driven by the large contributions from phonons, [12,21] carbon nanotube films can introduce a range of phonon scattering mechanisms that strongly reduce thermal conductivity. [22-24] This allows consideration of such disordered CNT films or mats for thermoelectric energy harvesting applications, and indeed these materials have recently shown promising thermoelectric figure-of-merit. [25,26] This is largely due to realization of theoretically predicted large Seebeck coefficients and large in-plane electronic conductivity when doped, and to dramatic reduction of thermal conductivity. This reduction is