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Control of interfacial electron transfer between electron transporting oxide semiconductors and molecular adsorbates in organic-inorganic hybrid solar cells is a research area of intense interest, with the poor optical harvesting in the red and near-IR (NIR) portion of the solar spectrum a significant limitation to device performance. We fabricate hybrid solar cells, using two new hemicyanine photosensitizers having different π-conjugation lengths that absorb sunlight from visible to NIR range, as well as unsymmetrical squaraine dye. These organic dyes are used not only as a photosensitizer, but also as electronic mediator for n-type TiO2 nanotube arrays, vertically oriented from the fluorine-doped tin oxide coated glass substrate, which are subsequently infiltrated with p-type regio-regular poly(3-hexyl thiophene 2,5 diyl), enabling broad-spectrum response. In general, the organic-dye-inorganic photovoltaic structure appears a promising method for harvesting a broad portion of the solar spectrum energy from a relatively simple photovoltaic device.