Shrinking volume, coupled with higher performance, microprocessors and integrated circuits have led to serious heat dissipation issues. In an effort to mitigate the excessive amounts of waste heat and ensure electronic survivability, heat sinks and spreaders are incorporated into heat generating device structures. This inevitability creates a thermal pathway through an interface. Thermal interfaces can possess serious thermal resistances for heat conduction. The introduction of a thermal interface material (TIM) can drastically increase the thermal performance of the component. Exceptional thermal properties of multiwall carbon nanotubes (MWCNTs) have spurred interest in their use as TIMs. MWCNTs inherently grow in vertically-oriented, high aspect ratio arrays, which is ideal in thermal interface applications because CNTs posses their superior thermal performance along their axis. In this paper, laser flash thermal characterization of sandwich‐bonded and cap‐screw‐bonded aluminum discs for both adhesive-infiltrated and “dry”, 100% MWCNT arrays, respectively. Thermal contact resistances as low as 18.1 mm2K/W were observed for adhesive‐infiltrated arrays and, even lower values, down to 10.583 mm2K/W were measured for “dry” MWCNT arrays. The improved thermal performance of the arrays compared to thermal adhesives and greases currently used in the electronics and aerospace industries, characterize MWCNT arrays as a novel, lighter‐weight, non‐corrosive replacement.

High performance/small package electronics create difficult thermal issues for integrated circuits. Challenges exist at material interfaces due to interfacial contact resistances. Multiwall carbon nanotube (MWCNT) arrays are considered to be excellent candidates for use as thermal interface materials (TIMs) due to outstanding thermal/mechanical properties. In this work, MWCNT array TIMs are analyzed in aluminum and carbon fiber composites via flash diffusivity analysis. The effect of TIM thickness, areal/bulk density, surface cleanliness, and volumetric packing fraction; along with the effect of substrate finish and interfacial contact pressure on thermal performance are analyzed. Trends show the best TIMs possess low thickness, high bulk density and packing fraction, and clean surfaces. Pressure dramatically increases thermal performance after establishing contact, with diminishing returns from additional pressure. Diffusivities approaching 40 mm2/s and 0.65 mm2/s are recorded for aluminum and composite systems. Oxygen plasma etching and high temperature annealing (“Graphitizing”) are investigated as methods to remove amorphous carbon from array surfaces. Graphitized TIMs report diffusivity improvements up to 53.8%. Three methods of incorporating MWCNTs into composites are attempted for thermal/mechanical property enhancement. Conductance calculations show increasing diffusivity without increasing thickness enhances thermal performance in composites. MWCNTs for mechanical property enhancement produce no change, or detrimental effects.