In the present work, MIL-101 nanoparticles (nano-MIL-101(Cr)) metal-organic framework (MOF) structure was synthesized by hydrothermal method, and characterized via Fourier transform infrared, X-ray diffraction, and scanning electron microscopy techniques. The optoelectronic application of MOFs was investigated for the first time. For this purpose, the dye-sensitized solar cells (DSSCs) consisting of the synthesized nano-MIL-101(Cr) impregnated photoanode (PA) was fabricated, and photovoltaic, photoelectric properties of them were investigated under different illumination intensities, and the obtained results were compared with reference one. The DSSC fabricated by impregnated PA showed better photovoltaic properties than reference one. It is obtained the power conversion efficiency (PCE) of about 0.828 and fill factor (ff) of 0.656 for the fabricated DSSC based on nano-MIL-101(Cr) impregnated PA under illumination power of 100 mW/cm(2) by AM1.5 G solar simulator. For the reference DSSC, PCE, and ff is about 0.468 and 0.28, respectively. The PCE of the fabricated device based on nano-MIL-101(Cr) is similar to 77% greater than the reference one. The improvement in the efficiency is because of good electrocatalytic activity, large pores, and high surface area of nano-MIL-101(Cr). The nano-MIL-101(Cr) can be used in organo-optoelectronic device fabrication to obtain better performance.