Two push-pull metal-free sensitizers with 5,11-dihydroindolo[3,2-b]carbazole derivatives as electron-donating groups and 4-(benzo[c][1,2,5]thiadiazol-4-ylethynyl)benzoic acid (BTZ) as electron-withdrawing unit, denoted by SK201 and SK202, were synthesized and used for fabrication of dye-sensitized solar cells (DSSCs). SK202 contains a thienyl group between the donor and acceptor, whereas in SK201 the donor and acceptor are connected directly by a single bond. Introduction of a thienyl group improved the planarity of the dye molecule, broadened the absorption spectrum, enhanced the molar extinction coefficient, increased the dye loading on TiO2, and accelerated interface electron transfer on TiO2. This fine tuning of dye structure improved the performances of DSSCs based on SK202 sensitizers and gave a power conversion efficiency (PCE) of 11.0% (J(SC) 16.5 mA cm(-2), V-OC 932 mV, and fill factor 71.7%), compared with that of 7.2% for SK201, under standard AM1.5G solar irradiation (100 mW cm(-2)) with a Co(II/III) complex based redox couple.