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Low-cost solar cells have been the subject of intensive research activities for over half century ago. More recently, dye-sensitized solar cells (DSSCs) emerged as a new class of low-cost solar cells that can be easily prepared. Natural-dye-sensitized solar cells (NDSSCs) are shown to be excellent examples of mimicking photosynthesis. The NDSSC acts as a green energy generator in which dyes molecules adsorbed to nanocrystalline layer of wide bandgap semiconductor material harvest photons. In this paper we investigate the structural, optical, electrical, and photovoltaic characterization of two types of natural dyes, namely, the Bahraini Henna and the Yemeni Henna, extracted using the Soxhlet extractor. Solar cells from both materials were prepared and characterized. It was found that the levels of open-circuit voltage and short-circuit current are concentration dependent. Further suggestions to improve the efficiency of NDSSC are discussed.