The synthesis of high-dielectric-constant (high-κ) dielectric materials and their integration with channel materials have been the key challenges in the state-of-the-art transistor architecture, as they can provide strong gate control and low operating voltage. For next-generation electronics, high-mobility two-dimensional (2D) layered semiconductors with dangling-bond-free surfaces and an atomic-thick thickness are being explored as channel materials to achieve shorter channel lengths and less interfacial scattering. Nowadays, the integration of high-κ dielectrics with high-mobility 2D semiconductors mainly relies on atomic layer deposition or transfer stacking, which may cause several undesirable problems, such as channel damage and interface traps. Here, we demonstrate the integration of high-mobility 2D semiconducting Bi