Robust, Self‐Healing, and Multi‐Use Poly(Urethane‐Urea‐Imide) Elastomer as a Durable Adhesive for Thermal Interface Materials

Abstract Currently, research on thermal interface materials (TIMs) is primarily focused on enhancing thermal conductivity. However, strong adhesion and multifunctionality are also important characteristics for TIMs when pursing more stable interface heat conduction. Herein, a novel poly(urethane‐urea‐imide) (PUUI) elastomer containing abundant dynamic hydrogen bonds network and reversible disulfide linkages is successfully synthesized for application as a TIM matrix. The PUUI can self‐adapt to the metal substrate surface at moderate temperatures (80 °C) and demonstrates a high adhesion strength of up to 7.39 MPa on aluminum substrates attributed its noncovalent interactions and strong intrinsic cohesion. Additionally, the PUUI displays efficient self‐healing capability, which can restore 94% of its original mechanical properties after self‐healing for 6 h at room temperature. Furthermore, PUUI composited with aluminum nitride and liquid metal hybrid fillers demonstrates a high thermal conductivity of 3.87 W m−1 K−1 while maintaining remarkable self‐healing capability and adhesion. When used as an adhesive‐type TIM, it achieves a low thermal contact resistance of 22.1 mm2 K W−1 at zero pressure, only 16.7% of that of commercial thermal pads. This study is expected to break the current research paradigm of TIMs and offers new insights for the development of advanced, reliable, and sustainable TIMs.