“…Time-domain thermoreflectance (TDTR), a technique with ultrahigh temporal and spatial resolutions, has been widely applied to measure the thermal properties of both bulk materials and nanostructured materials. , Meanwhile, TDTR is a nondestructive and noncontact pump–probe technique to study heat transport across heterogeneous interfaces, merely by depositing a metal transducer layer on the target material surface. Particularly, assisted by the equipped high-resolution optical microscopy, TDTR can ensure precise testing locations. , In addition, by combining the interface microstructure and measured thermal boundary conductance ( G ), the single effect of interface characteristics on electron and phonon scattering as well as their coupling behaviors can be analyzed. − For instance, for widely studied heat transport across metal/nonmetal interfaces, a large number of studies have demonstrated that electron–phonon coupling at the metal side (the first heat transport pathway) is closely related to the metal orientation and defects near the interface, , and thermal resistance generated in this pathway ( R 1 ) intrinsically is determined by relaxation time (τ) of electrons and phonons. Following this process, the phonon–phonon coupling (the second heat transport pathway) between metal and nonmetal happens, and this coupling process is mainly influenced by defects at the interface, interface orientation, interface compositions, and interfacial bonding .…”