Organic/inorganic hybrid materials are utilized extensively as gate dielectric layers in organic thin‐film transistors (OTFTs). However, inherently low dielectric constant of organic materials and lack of a reliable deposition process for organic layers hamper the broad application of hybrid dielectric materials. Here, a universal strategy to synthesize high‐k hybrid dielectric materials by incorporating a high‐k polymer layer on top of various inorganic layers generated by different fabrication methods, including AlOx and HfOx, is presented. Those hybrid dielectrics commonly exhibit high capacitance (>300 nF·cm–2) as well as excellent insulating properties. A vapor‐phase deposition method is employed for precise control of the polymer film thickness. The ultralow‐voltage (<3 V) OTFTs are demonstrated based on the hybrid dielectric layer with 100% yield and uniform electrical characteristics. Moreover, the exceptionally high stability of OTFTs for long‐term operation (current change less than 5% even under 30 h of voltage stress at 2.0 MV·cm–1) is achieved. The hybrid dielectric is fully compatible with various substrates, which allows for the demonstration of intrinsically flexible OTFTs on the plastic substrate. It is believed that this approach for fabricating hybrid dielectrics by introducing the high‐k organic material can be a promising strategy for future low‐power, flexible electronics.