A novel concept "D-A-pi-A" organic sensitizer instead of traditional D-pi-A ones is proposed. Remarkably, the incorporated low bandgap, strong electron-withdrawing unit of benzothiadiazole shows several favorable characteristics in the areas of light-harvesting and efficiency: i) optimized energy levels, resulting in a large responsive range of wavelengths into NIR region; ii) a very small blue-shift in the absorption peak on thin TiO2 films with respect to that in solution; iii) an improvement in the electron distribution of the donor unit to distinctly increase the photo-stability of synthetic intermediates and final sensitizers. The stability and spectral response of indoline dye-based DSSCs are improved by the strong electron-withdrawing benzothiadizole unit in the conjugation bridge. The incident-photon-conversion effi ciency of WS-2 reaches nearly 850 nm with a power conversion effi ciency as high as 8.7% in liquid electrolyte and 6.6% in ionic-liquid electrolyte.