Improvements in thermal interface materials (TIMs) can enhance heat transfer in electronics packages and reduce high temperatures. TIMs are generally composed of highly conductive particle fillers and a matrix that allows for good surface wetting and compliance of the material during application. Two types of TIMs are tested based on the addition of carbon nanotubes (CNTs): one mixed with a commercial TIM product and the other only CNTs and silicone oil. The materials are tested using an in-house apparatus that allows for the simultaneous measurement of temperature, pressure, heat flux, and TIM thickness. Results show that addition of large quantities of CNTs degrades the performance of the commercial TIM, while the CNT-silicone oil mixtures showed improved performance at high pressures. Thickness and pressure measurements indicate that the CNT-thermal grease mixtures are more compliant, with a small increase in bulk thermal conductivity over the range of tested pressures.