Organic semiconductors are emerging as a viable alternative to amorphous silicon in a range of thin‐film transistor devices. With the possibility to formulate these p‐type materials as inks and subsequently print into patterned devices, organic‐based transistors offer significant commercial advantages for manufacture, with initial applications such as low performance displays and simple logic being envisaged. Previous limitations of both air stability and electrical performance are now being overcome with a range of both small molecule and polymer‐based solution‐processable materials, which achieve charge carrier mobilities in excess of 0.5 cm2 V−1 s−1, a benchmark value for amorphous silicon semiconductors. Polymer semiconductors based on thienothiophene copolymers have achieved amongst the highest charge carrier mobilities in solution‐processed transistor devices. In this Progress Report, we evaluate the advances and limitations of this class of polymer in transistor devices. Thienothiophene semiconducting polymers can exhibit a planar backbone conformation, leading to highly crystalline structures, often with good orientation and inter‐grain alignment. This thin‐film microstructure is optimal in achieving high charge‐carrier mobilities in organic field‐effect transistors.