A series of new D-D-π-A-type indol-triarylamine sensitizers were designed and evaluated by the theoretical calculations. Based on the exciting results of calculation, they were synthesized and used as the sensitizers for DSSCs. The results indicated that the incorporation of indole derivatives and TPA skeleton made the new dyes possessing excellent non-planarity, optical and electrochemical properties, thermo-stability and relative high melting point and therefore performed well as expected as the dyes of a DSSC.