As the feature size of integrated circuit devices is shrinking to sub-7 nm node, the chip
power dissipation significantly increases and mainly converted to the heat. Vertically Aligned Carbon
Nanotube arrays (VACNTs) have a large number of outstanding properties, such as high axial thermal
conductivity, low expansion coefficient, light-weight, anti-aging, and anti-oxidation. With a dramatic
increment of chip temperature, VACNTs and their composites will be the promising materials as Thermal
Interface Materials (TIMs), especially due to their high thermal conductivity. In this review, the synthesis,
transfer and potential applications of VACNTs have been mentioned. Thermal Chemical Vapor
Deposition (TCVD) has been selected for the synthesis of millimeter-scale VACNTs. After that, they are
generally transferred to the target substrate for the application of TIMs in the electronics industry, using the
solder transfer method. Besides, the preparation and potential applications of VACNTs-based composites
are also summarized. The gaps of VACNTs are filled by the metals or polymers to replace the low
thermal conductivity in the air and make them free-standing composites films. Compared with VACNTs-
metal composites, VACNTs-polymer composites will be more suitable for the next generation
TIMs, due to their lightweight, low density and good mechanical properties.