Two new metal-free organic dyes which consist of a saddle-shaped tetraindole donor, a cyanoacrylic acid acceptor/anchoring group and a thiophene or bithiophene π-bridge have been successfully designed and synthesized for dye-sensitized solar cells. The two dyes showed good photoelectric properties, and the saddle-shaped structure of the tetraindole unit was found to be favorable for preventing intermolecular aggregation and enhancing the photovoltage. The two tetraindole-based dyes exhibited good photovoltaic performances in solar cells. An efficiency up to 6.46% with a high open-circuit photovoltage of 762 mV was achieved for the dye JY15 with a 2,2′-bithiophene moiety as the π-bridge using an iodine electrolyte under standard conditions.