Low-voltage operation is one of the prerequisites for the practical applications of the organic thin-film transistors (OTFTs). Up to date, the most reported low-voltage operatable OTFTs use a bottom-gate structure, and are fabricated by several different technologies in the whole process, in which the organic semiconductors and/or gate dielectrics are prepared in the expensive vacuum equipment. The simple fabricating technologies and fewer processes can better demonstrate the inherent advantages, and enhance the commercial competitiveness of OTFTs. Here, we propose a strategy to fabricate the binary polymers gate dielectric by one-step spin-coating in the top-gate structured flexible OTFTs, by which not only the device performances are prominently improved, but also the fabricating process of the OTFTs is minimized. As a result, the flexible OTFTs exhibit a high mobility over 0.5 cm2 Vs−1, low threshold voltage near to −0.5 V, and excellent mechanical bending durability with a very slightly performances degradation after the tensile and compressive bending at a small curvature radius of 3.0 mm over 1000 cycles.