AbstractWearable haptic devices are developed as key components to enhance the highly immersive metaverse experience. However, conventional haptic devices enabling the sensation and interaction with virtual objects are often constrained by their bulky design, tethered operation, and physical interference with the skin, especially when integrated with human hands. In this study, a cross‐interface modification process that achieves the conversion of multilayered silk fibroin films from rigid to soft is reported. This modification is favorable for applications involving large angles and multiple degrees of freedom motions. By applying electrical current through silk‐based electrodes and utilizing a self‐designed circuit, virtual tactile sensations can be generated on the entire palm. The high flexibility, stretchability, tailorable modulus, and water permeability of silk substrates enable the electrotactile devices to maintain their functionalities without impeding fine movements and natural tactile sensations in the hand. This compact electrotactile system serves as a user's new interactive terminal through wireless communications. The intimate contact interfaces reduce the unstable adhesion commonly encountered in electrotactile applications, ensuring consistent sensation during hand motions. These materials design methods and integrated systems represent a significant advancement in fabricating and integrating large‐area soft electronics.