Elastomeric polymer materials are of interest due to their stretchability, low‐temperature processing, and scalability. In addition, the incorporation of 2D materials can further enhance the dielectric properties and capacitance of elastic polymer materials, thereby reducing the driving voltage and energy consumption. In this study, titanium dioxide (TiO2) nanosheets are cross‐linked with nitrile butadiene rubber using thiol‐ene click chemistry, which leads to the preparation of nanocomposite dielectric films with stretchability and high dielectric constant. Furthermore, by controlling the doping amount of the nanosheets, it is observed that the capacitance of the nanocomposite films increases from 25.61 to 684.67 nF cm−2, and the dielectric constant increases from 14.96 to 161.98. Finally, the stretchable nanocomposite films exhibit good insulating properties even at 50% strain. In this study, insight is provided into the potential of in situ cross‐linking between elastic polymer materials and 2D materials to produce high‐k dielectric materials with both stretchability and high insulating properties.
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