Transition metal dichalcogenides like MoS 2 have been considered as crucial channel materials beyond silicon to continuously advance transistor scaling down owing to their two-dimensional structure and exceptional electrical properties. However, the undesirable interface morphology and vibrational phonon frequency mismatch between MoS 2 and the dielectric layer induce low thermal boundary conductance, resulting in overheating issues and impeding electrical performance improvement in the MoS 2 field-effect transistors. Here, we employed hybrid high-k dielectric layers of Al 2 O 3 /HfO 2 to simultaneously reduce the interfacial thermal resistance and improve device electrical performance. The enhanced contact, greater vibrational phonon overlapping region, and stronger interfacial bonding force between the top Al 2 O 3 layer and MoS 2 promote the heat removal efficiency across the interface to the substrate. Under the same input power density, the temperature profile of the MoS 2 transistor on the Al 2 O 3 /HfO 2 has been largely reduced compared to that of the device on HfO 2 , with a maximum reduction of 49.5 °C. In addition, the field-effect mobility and current of MoS 2 devices on the Al 2 O 3 /HfO 2 high-k dielectric layers have been significantly improved, attributed to the depressed electron scattering and trap states at the interface. The design of the hybrid high-k dielectric layers provides an efficient solution to simultaneously improve the thermal and electrical performance of the two-dimensional devices. KEYWORDS: thermal dissipation, thermal boundary conductance, MoS 2 field-effect transistor, high-k dielectric layer, Al 2 O 3 /HfO 2 , temperature profile