Polymer-based
thermal interface materials integrated with excellent
stretchability and simultaneously high thermal conductivity would
be of great use in the thermal management of next-generation chips
featuring higher power density and a larger packaging size. However,
combining thermal conductivity and stretchability in the same material
is fundamentally challenging. Herein, in view of the important role
of filler/polymer interface, we report a stretchable thermal interface
material by tailoring chain relaxation through incorporating macromolecular
coupling agent at the aluminum/silicone interface. Thanks to the interfacial
relaxation effect, the aluminum/silicone thermal interface material
exhibits a large stretchability (117%) and a high thermal conductivity
(5.90 W m–1 K–1) at the aluminum
weight fraction of 91 wt %. Moreover, these materials show great heat
dissipation performance in practical applications, which we demonstrated
by rapid heat dissipation in LED and chip. This strategy will provide
an avenue to implement interface design for high-performance thermal
interface materials for high-performance applications, such as high-performance
computing, the Internet of Things, 5G networking, and artificial intelligence
computing.