In order to improve thermal interface material (TIM), vertically aligned carbon nanotube (VACNT) arrays were synthesized by the chemical vapor deposition method, and then transferred by dipping in hydrofluoric acid (HF acid) solution to get a free standing VACNT array. Different TIM samples with sandwiched structures were fabricated by inserting the free standing VACNT arrays between two copper plates with and without bonding materials. The laser flash analysis method was applied to measure the overall thermal conductivity of these samples. Results show that: compared with two copper plates in direct contact, thermal conductivity of samples only with VACNT arrays as TIM can be enhanced about 142%–460% depending on the thickness of VACNT arrays. Conventional TIM made up of thermal paste (TG-550 with thermal conductivity of 5 W/mK) and a thermal pad (TP-260 US with thermal conductivity of 6 W/mK) was used as a bonding material between copper plates and VACNT arrays, thermal conductivity has been shown to further improve with the highest values at 8.904 W/mK and 10.17 W/mK corresponding to the different bonding materials and different thicknesses of VACNT arrays used. Results also show that the thicker the VACNT array is when used as a TIM, the lower the overall thermal conductivity of the corresponding samples. This lower thermal conductivity caused by more defects in amorphous carbon of thicker VACNT arrays and lower density of the corresponding sandwiched samples.

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