With the miniaturization and integration of wearable electronics, there are some serious problems such as signal crosstalk and high power consumption that restrict its development. Active‐matrix thin‐film transistors (TFTs) with high permittivity (high‐k) insulator layer provide a promising opportunity for reducing signal crosstalk and power consumption of wearable electronics. Here, we propose a simple and cost‐effective gradient heating‐up strategy to prepare high‐k zirconium dioxide (ZrO 2)‐based dielectric films. Amorphous ZrO 2 films annealed at 400°C exhibits a high transmittance and a high dielectric properties of a relative low leakage current (10‐8 A/cm2 ) and large capacitance density of 215 nF/cm2 . To meet requirements of flexible wearable electronics, ZrO 2‐organic polymer hybrid dielectric film was further developed. A smooth surface morphology (Sa=0.478 nm) and good dielectric performance (~10‐8 A/cm2 ) of ZrO 2‐based hybrid film was obtained at 250°C, which can promote the development of flexible TFT and extend the application scenarios of wearable electronics.