Synthesis and investigation of new donor-acceptor conjugated N-(5-arylazothiazol-2-yl)-2-aminothiophene derivatives with the aim to elucidate the contribution of their interaction with solvent molecules upon intramolecular charge transfer for their potential solar cells application. The UV-visible and emission spectra measurements indicated that the properties of the synthesized dyes had a significant effect on the visible absorption and emission maxima. The effect of the donor and acceptor groups were studied for the nonlinearity based on their HOMO-LUMO band gap energy. The dye-sensitized solar cells (DSSCs) were assembled by using the newly synthesized aryl thiazolyl-thiophene dyes as sensitizers. The promising results of J(SC) (2.46 × 10(-2) and 4.07 × 10(-2) mA/cm(2)), the V(OC) (0.429 V and 0.426 V) and the FF (0.66 %) values obtained comparing with other organic and natural sensitizer were due to the better interaction between the carboxyl and carbonyl groups of aryl azo molecule attached to the thiazolyl nucleus and the surface of TiO(2) porous film.