Enhanced Thermal Transport across Self‐Interfacing van der Waals Contacts in Flexible Thermal Devices

Abstract Minimizing the thermal contact resistance (TCR) at the boundary between two bodies in contact is critical in diverse thermal transport devices. Conventional thermal contact methods have several limitations, such as high TCR, low interfacial adhesion, a requirement for high external pressure, and low optical transparency. Here, a self‐interfacing flexible thermal device (STD) that can form robust van der Waals mechanical contact and low‐resistant thermal contact to planar and non‐planar substrates without the need for external pressure or surface modification is presented. The device is based on a distinctive integration of a bioinspired adhesive architecture and a thermal transport layer formed from percolating silver nanowire (AgNW) networks. The proposed device exhibits a strong attachment (maximum 538.9 kPa) to target substrates while facilitating thermal transport across the contact interface with low TCR (0.012 m² K kW⁻¹) without the use of external pressure, thermal interfacial materials, or surface chemistries.