Advanced Materials, 22 (2010), 37, 4198 Nature Chemistry, 3 (2011), 359• Chemical Reviews, 111 (2011), 4833 organic synthesis allows for the preparation of materials “à la carte”. We have shown that organic fieldeffect transistors (OFETs) based on TTFs exhibit excellent OFET mobility (up to 6 cm2/Vs) as well as easy processability. Our recent work is related to explore the influence of crystal structure, polymorphism, electronic structure and device configuration and interfaces in TTF OFETs (Figure 2).