A series of new organic dyes comprising different amines as electron donors, 2-(6-substituted-anthracen-2-yl)-thiophene as the π-conjugated bridge, and cyanoacrylic acid group as an electron acceptor and anchoring group, have been synthesized. There exists charge transfer transition from arylamine and anthracene to the acceptor in these compounds, as evidenced from the photophysical measurements and the computational results. Under one sun (AM 1.5) illumination, dye-sensitized solar cells (DSSCs) using these dyes as the sensitizers exhibited efficiencies ranging from 1.62% to 2.88%, surpassing that using 9,10-difunctionalized anthracene-based sensitizer.