Two-dimensional (2D) semiconductors such as monolayer MoS₂ hold significant promise for advancing nanoelectronics. However, integrating high-k dielectrics with 2D semiconductors to achieve high performance devices remains a challenge. In this talk, I will present our understanding of designing high-performance interfaces between high-k dielectrics and 2D MoS₂. First, we demonstrate that hydrogenation is an effective method for passivating dangling bonds at the interface between conventional high-k dielectrics and MoS₂, in which hydrogenation selectively occurs on high-k dielectrics such as Si₃N₄ and HfO₂ without affecting the MoS₂. Second, we introduce a data-driven approach to expedite the discovery of inorganic molecular crystals (IMCs) as high-k dielectrics. From enormous candidates in Materials Project, we identify 9 IMCs as the promising high-k dielectrics for 2D semiconductors. These findings advance the understanding of integrating high-k dielectrics with 2D semiconductors and could be useful for the development of a wide range of 2D electronic and optoelectronic devices.