Adaptive Self‐Organization of Nanomaterials Enables Strain‐Insensitive Resistance of Stretchable Metallic Nanocomposites

Abstract Highly conductive and stretchable nanocomposites are promising material candidates for skin electronics. However, the resistance of stretchable metallic nanocomposites highly depends on external strains, often deteriorating the performance of fabricated electronic devices. Here, a material strategy for the highly conductive and stretchable nanocomposites comprising metal nanomaterials of various dimensions and a viscoelastic block‐copolymer matrix is presented. The resistance of the nanocomposites can be well retained under skin deformations (<50% strain). It is demonstrated that silver nanomaterials can self‐organize inside the viscoelastic media in response to external strain when their surface is conjugated with 1‐decanethiol. Distinct self‐organization behaviors associated with nanomaterial dimensions and strain conditions are found. Adopting the optimum composition of 0D/1D/2D silver nanomaterials can render the resistance of the nanocomposites insensitive to uniaxial or biaxial strains. As a result, the resistance can be maintained with a variance of < 1% during 1000 stretching cycles under uniaxial and biaxial strains of <50% while a high conductivity of ≈31 000 S cm −1 is achieved.