Polymer nanowire (NW) organic field-effect transistors (OFETs) integrated on highly aligned large-area flexible substrates are candidate structures for the development of high-performance flexible electronics. This work presents a universal technique, coaxial focused electrohydrodynamic jet (CFEJ) printing technology, to fabricate highly aligned 90-nm-diameter polymer arrays. This method allows for the preparation of uniformly shaped and precisely positioned nanowires directly on flexible substrates without transfer, thus ensuring their electrical properties. Using indacenodithiophene-co-benzothiadiazole (IDT-BT) and poly(9,9-dioctylfluorene-co-benzothiadiazole) (F8-BT) as example materials, 5 cm2arrays were prepared with only minute size variations, which is extremely difficult to do using previously reported methods. According to 2D-GIXRD analysis, the molecules inside the nanowires mainly adopted face-on π-stacking crystallite arrangements. This is quite different from the mixed arrangement of thin films. Nanowire-based OFETs exhibited a high average hole mobility of 1.1 cm2V−1s−1and good device uniformity, indicating the applicability of CFEJ printing as a potential batch manufacturing and integration process for high-performance, scalable polymer nanowire-based OFET circuits. This technique can be used to fabricate various polymer arrays, enabling the use of organic polymer semiconductors in large-area, high-performance electronic devices and providing a new path for the fabrication of flexible displays and wearable electronics in the future.