A D-pi-A dye (KM-1) incorporating cyanobenzoic acid as a new acceptor/anchoring group has been synthesized for dye-sensitized solar cells (DSCs) with a high molar extinction coefficient of 66 700 M-1 cm(-1) at 437 nm. Theoretical calculations show that the hydrogen bond between -CN and surface hydroxyl leads to the most stable configuration on the surface of TiO2. In addition, the adsorption of the dye on TiO2 follows a Brunauer-Emmett-Teller (BET) isotherm. Multilayer adsorption of KM-1 on TiO2 seems to take place particularly at higher dye concentrations. DSC device using KM-1 reached a maximum incident photon-to-current conversion efficiency (IPCE) of 84%, with a solar to electric power conversion efficiency (PCE) of 3.3% at AM1.5 G illumination (100 mW cm(-2)). This new type of anchoring group paves a way to light harvesting with strong binding to the metal oxide surface. design new dyes that combine good visible