Mengjie Li, Wenwu Jiang, Huasong Qin, Wengen Ouyang, Chun Li
Precise control of interfacial thermal resistance (ITR) is essential for thermal management in van der Waals (vdW) devices. Here, we report a counterintuitive temperature-dependent reversal of ITR in twisted PtX2 (X = S, Se, Te) interfaces. At near-commensurate small twist angles, elevated temperatures enhance anharmonic scattering, suppressing direct phonon transmission and dramatically increasing ITR. In contrast, at incommensurate large twist angles, heat transport paradoxically improves because direct transmission is inherently limited by structural mismatch, allowing thermally activated inelastic vibrational pathways to dominate and reduce ITR. Spectral energy density and spectral heat current analyses confirm that this reversal arises from a dynamic competition between the degradation of direct channels and the activation of inelastic channels. The phenomenon extends universally to other vdW architectures, including graphene and MoS2, establishing twist-temperature co-regulation as an effective route for tailoring interfacial thermal transport in vdW materials.