Two indole-based organic dyes were conveniently prepared and well characterized. The triphenylamine or carbazole moieties were bonded to the indole group acting as a potential electron donor, which can tune the HOMO and LUMO levels of the resultant dye, and another triphenylamine or carbazole group was linked to the pyrrole ring on the nitrogen atom, which was expected to suppress the aggregation of the dye in the solid state to some degree. These two dyes were utilized as dye sensitizers in dye-sensitized solar cells and demonstrated efficient photon-to-electron conversion properties.