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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.