Seven flavylium salt dyes were employed for the first time assensitizersfordye-sensitizedsolarcells(DSSCs). The theoretical and experimental wavelengths of the maximum absorbances, the HOMO and LUMO energy levels, the coefficients, the oscillator strengths and the dipole moments are calculated for thesesyntheticdyes. The introduction of a donor group in the flavylium molecular structure was investigated. Photophysical and photoelectrochemical measurements showed that some of thesesyntheticanaloguesofanthocyaninsare very promising for DSSC applications. The best performance was obtained by a DSSC based on the novel compound 7-(N,N-diethylamino)-3',4'-dihydroxyflavylium which produced a 2.15%solarenergy-to-electricity conversion efficiency, under AM 1.5 irradiation (100 mW cm(-2)) with a short-circuit current density (J(sc)) of 12.0 mA cm(-2), a fill factor of 0.5 and an open-circuit voltage (V(oc)) of 0.355 V; its incident photocurrent efficiency of 51% at the peak of the visible absorption band of the dye is remarkable. Our results demonstrated that the substitution of a hydroxylic group with a diethylamine unit in position 7 of ring A of the flavylium backbone expanded the π-conjugation in the dye and thus resulted in a higher absorption in the visible region and is advantageous for effective electron injection from the dye into the conduction band of TiO2.