Triazoloisoquinoline-based organic dyestuff was synthesized and used in the fabrication of dye-sensitized solar cells (DSSCs). After co-sensitization with ruthenium complex, triazoloisoquinoline-based organic dyestuff overcomes the deficiency of ruthenium dyestuff absorption in the blue part of the visible spectrum. The incident photon-to-electron conversion efficiency (IPCE) of cis-dithiocyanate-N,N'-bis-(4-carboxylate-4-tetrabutyl ammoniumcarboxylate-2,2'-bipyridine) ruthenium(II) (N719) at shorter wavelength regions (similar to 350-500 nm) is 35 %. After addition of triazoloisoquinoline-based dyestuff for co-sensitization, the IPCE at 350-500 nm increased significantly. This can be attributed to the increased photocurrent of the cells, which improves the dye-sensitized photoelectric conversion efficiency. After optimization of the cells, an energy conversion efficiency of 8.83 % was achieved using an 12 + 4 mu m TiO2 electrode, under simulated solar illumination (AM 1.5G). As a consequence, this low molecular weight organic dyestuff is a promising candidate as a co-adsorbent and co-sensitizer for highly efficient DSSCs.