Abstract: | Stretchable electronic devices should be enabled by the smart design of materials and architectures because their commercialization is limited by the tradeoff between stretchability and electrical performance limits. In this study, thin‐film transistors are fabricated using strategies that combine the unit process of a novel hybrid gate insulator and low‐temperature indium gallium tin oxide (IGTO) channel layer and a stress‐relief substrate structure. Novel hybrid dielectric films are synthesized and their molecular structural configurations are analyzed. These films consist of a polymer poly(4‐vinylphenol‐co‐methylmethacrylate)], cross‐linkers having different binding structures 1,6‐bis(trimethoxysilyl)hexane (BTMSH), dodecyltrimethoxysilane, and poly(melamine‐co‐formaldehyde)], and an inorganic zirconia component (ZrOx). The hybrid film with BTMSH cross‐linker and 0.2 M ZrOx exhibits excellent insulating properties as well as mechanical stretchability. IGTO transistors fabricated on polyimide‐coated glass substrates are transferred to the rubber substrate to offer stretchability of the transistor pixelated thin‐film transistors. IGTO transistors fabricated on stretchable substrates using these strategies show promising electrical performance and mechanical durability. After 200 stretchability test cycles under uniaxial elongation of approximately 300%, the IGTO transistor still retains a high carrier mobility of 21.7 cm2 V?1 s?1, a low sub‐threshold gate swing of 0.68 V decade?1 and a high ION/OFF ratio of 2.0 × 107. |