Metal-organic frameworks (MOFs) are multifunctional inorganic-organic hybrid 3D networks that can be fine tuned through various modifications, making them semiconductive and highly adaptable in many applications.In this study, the semiconducting behavior of a notable MOF, Co-MOF-74 was enhanced, via post-synthetic modifications.Electron-rich guest mols.; aniline, m-toluidine, p-toluidine, o-anisidine, and p-anisidine were encapsulated into the honeycomb-shaped channels in Co-MOF-74 structure using the vapor phase encapsulation method.The successful synthesis of Co-MOF-74 was confirmed through powder X-ray diffraction, showing major diffraction peaks at approx. 6.7° and 11.7°, corresponding to the (2-10) and (300) crystal planes, resp.Fourier-transform IR anal. proved the successful encapsulation of the guest mols., as evidenced by band shifts towards lower wavenumber values in the 1700-1300 cm-1 region.The encapsulation of guest mols. significantly reduced the bandgap of Co-MOF-74, from 2.72 eV for the pristine Co-MOF-74 to 1.89, 2.56, 2.54, 2.14, and 1.92 eV upon encapsulation with aniline, m-toluidine, p-toluidine, o-anisidine, and p-anisidine, resp. and flat band potentials reduced, and carrier concentrations improved.These results highlight the potential of using Co-MOF-74 for enhanced semiconducting applications through targeted guest mol. encapsulation.Hence, to improve the cost-effectiveness of dye-sensitized solar cells, modified Co-MOF-74 systems were applied as both semiconducting and sensitizing materials in fabricating MOF-sensitized solar cells (MSSC).Upon electro-polymerization via cyclic voltammetry anal., the MSSC efficiencies improved to 0.01 %, indicating promising advancements in the efficiency of MOF-sensitized solar cells.