In this study, we have been synthesized the dielectric layer using pure organic and organic-inorganic hybrid precursor on flexible substrate for improving of the organic thin film transistors (OTFTs) and, design and fabrication of organic thin-film transistors (OTFTs) using small-molecule organic semiconductors with pentacene as the active layer with record device performance. In this work OTFT test structures fabricated on polymerized substrates were utilized to provide a convenient substrate, gate contact, and gate insulator for the processing and characterization of organic materials and their transistors. By an adhesion development between gate metal and PI substrate, a PI film was treated using $O_2$ and $N_2$ gas. The best peel strength of PI film is 109.07 gf/mm. Also, we have studied the electric characteristics of pentacene field-effect transistors with the polymer gate-dielectrics such as cyclohexane and hybrid (cyclohexane+TEOS). The transistors with cyclohexane gate-dielectric has higher field-effect mobility, $mu_{FET}=0.84;cm^2/v_s$, and smaller threshold voltage, $V_T=-6.8;V$, compared with the transistor with hybrid gate-dielectric.