There is an increasing demand for freeform stretchable display technologies capable of overcoming spatial limitations in next-generation platforms such as augmented reality (AR) and virtual reality (VR). To realize such stretchable displays, all constituent materials—including semiconductors, electrodes, insulators, and substrates—must exhibit sufficient mechanical elasticity. To date, stretchable gate insulators have primarily relied on organic polymers such as poly(4-vinylphenol-co-methyl methacrylate) (PVP-co-PMMA). However, their practical application is significantly limited by poor electrical properties, including low dielectric constant and instability. In this work, we propose a novel gate insulator structure that minimizes the use of solution-based processes, which often suffer from poor uniformity and may damage underlying layers during fabrication. The proposed structure integrates the advantages of both organic and inorganic materials by employing a hybrid configuration. Specifically, high-k HfO₂ thin films are deposited on both the top and bottom of an organic layer composed of PVP-co-PMMA, poly(melamine-co-formaldehyde) (PMF) as a crosslinking agent, and propylene glycol monomethyl ether acetate (PGMEA) as a solvent. This inorganic–organic–inorganic structure effectively compensates for the inherent electrical limitations of organic materials. As a result, the fabricated thin-film transistors (TFTs) exhibit improved electrical performance and reliability compared to devices employing a single organic gate insulator.