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Mobility is an important parameter to estimate the performance of organic thin‐film transistors, one of the key factors affecting the mobility is the first several semiconductors molecular layers near the insulator surface. A strategy is proposed to introduce aromatic‐rings in the gate insulating layer to modulate the growth of pentacene, thus a series of aryl group containing polymers by reversible‐addition‐fragmentation chain‐transfer polymerization is synthesized for the preparation of organic thin‐film transistor insulators. The semiconductor layer is evaporated on the polymer insulators at room temperature. As the inducing function of the aromatic ring, greater weak interactions between dielectric materials and semiconductors by simulation, which makes the initial pentacene layer weak epitaxial growth, therefore pentacene could form better morphology, especially larger crystal domains and uniform thin‐film continuity. The results show that precision design and synthesis of polymer insulator layers provide new methods to achieve high performance of organic thin‐film transistors with easier fabricating process. [ABSTRACT FROM AUTHOR]