Two new D–D–π–π–A type stable organic sensitizers, DT3 and DW3, were successfully synthesized for dye-sensitized solar cells (DSSCs). DT3 displayed η values of 10.03% and 8.05% in liquid and quasi-solid-state DSSCs, respectively, under standard global 1.5 solar conditions, offering an example achieving the highest efficiency to date in quasi-solid-state DSSCs based on pure organic dyes.