Compounds incorporating the tetrathiafulvalene (TTF) donor unit and one or two cyanoethynylethene (CEE) acceptor units were prepared by Knoevenagel condensations of highly unstable, TTF-linked propargylic aldehyde or ketone derivatives. The resulting TTF-CEEs are very strong chromophores with low-energy end-absorptions beyond 900 nm. The molecules experience reversible oxidations of the TTF unit, and the optical properties of the oxidised species were elucidated by spectroelectrochemistry.