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Abstract The difficulty of achieving ohmic contacts is a long‐standing challenge for the development and integration of devices based on 2D materials, due to the large mismatch between their electronic properties and those of both traditional metal‐based and van der Waals (vdWs) electrodes. Research has focused primarily on the electronic energy band alignment, while the effects of momentum mismatch on carrier transport across the vdWs gaps are largely neglected. Graphene‐silicon junctions are utilized to demonstrate that electron momentum distribution can dominate the electronic properties of vdWs contacts. By judiciously introducing scattering centers at the interface that provide additional momentum to compensate the momentum mismatch, the junction conductivity is enhanced by more than three orders of magnitude, enabling the formation of high‐quality ohmic contacts. The study establishes the framework for the design of high‐performance ohmic vdWs contacts based on both energy and momentum matching, which can facilitate efficient heterogeneous integration of 2D–3D systems and the development of post‐CMOS architectures. 

Abstract Van der Waals semiconductors (vdWS) offer superior mechanical and electrical properties and are promising for flexible microelectronics when combined with polymer substrates. However, the self‐passivated vdWS surfaces and their weak adhesion to polymers tend to cause interfacial sliding and wrinkling, and thus, are still challenging the reliability of vdWS‐based flexible devices. Here, an effective covalent vdWS–polymer lamination method with high stretch tolerance and excellent electronic performance is reported. Using molybdenum disulfide (MoS₂)and polydimethylsiloxane (PDMS) as a case study, gold–chalcogen bonding and mercapto silane bridges are leveraged. The resulting composite structures exhibit more uniform and stronger interfacial adhesion. This enhanced coupling also enables the observation of a theoretically predicted tension‐induced band structure transition in MoS₂. Moreover, no obvious degradation in the devices’ structural and electrical properties is identified after numerous mechanical cycle tests. This high‐quality lamination enhances the reliability of vdWS‐based flexible microelectronics, accelerating their practical applications in biomedical research and consumer electronics.