Carbon nanotube (CNT) forests or sheets coated and/or bonded at room temperature with one or more coatings were measured to produce thermal resistances that are on par with conventional metallic solders. These results were achieved by reducing the high contact resistance at CNT tips and/or sidewalls, which has encumbered the development of high-performance thermal interface materials based on CNTs. Resistances as low as 4.9±0.3 mm2−K/W were achieved for the entire polymer-coated CNT interface structure.