Research New: The versatile 1,3-dithiole (DT) ring system probably holds the record among heterocyclic systems for the most widespread use in modern materials science. Interest in derivatives of DT and the 1,3-dithiolium cation DT+ was boosted in the past by the discovery of metal-like conductivity in the charge-transfer complex TTF-TCNQ and superconductivity in cation radical salts of TMTSF and BEDT-TTF. The authors examine some of the new functionalized pi-donor systems based on the TTF framework and comment on possible applications as sensors, molecular shuttles, organic ferromagnets and electroactive Langmuir-Blodgett films.