Correlation between the Cross-Plane Thermal and Electrical Conductance in Randomly Stacked MoS₂

van der Waals (vdW) interface is a critical component in the performance of flexible devices, such as electronics, thermal, and thermoelectric devices. Recent advances in interface design with two-dimensional (2D) materials have allowed for studying various controlled interface properties. Understanding the heat and charge transport correlation is essential for optimizing flexible device performance. However, due to experimental limitations, the correlation between the heat and charge transport characteristics across 2D vdW interfaces has not yet been elucidated. Here, we revealed the thermal and electrical conductance across four randomly stacked MoS₂ layers. The simultaneous determination of cross-plane thermal and electrical conductance can be achieved using time-domain thermoreflectance measurements using Au as a metal transducer. A linear correlation between thermal and electrical conductance was observed by vacuum annealing, and such behavior can be understood by the change in interlayer distance from theoretical calculations. Our study offers insights into thermal management for nanodevices using stacked 2D materials.