In this study, we report the efficient removal of organic dyes from aqueous solutions using a newly synthesized pyrene-appended Zn(II)-based metal-organic framework (MOF), ZnSiF6Pyrene MOF, with the chemical formula CHFNSiZn·4(CHCl). The MOF was synthesized through a facile method at room temperature using a dipyridylpyrene ligand and ZnSiF metal source, resulting in a highly crystalline structure with pyrene functional groups forming the framework. The synthesized MOF was characterized using various analytical techniques, including Fourier-transform infrared spectroscopy (FT-IR), powder X-ray diffraction (PXRD) analysis, and scanning electron microscopy (SEM). Thermal stability was assessed using thermogravimetric analysis (TGA), while the surface area of the MOF was determined using a Brunauer-Emmett-Teller (BET) surface analyzer. Furthermore, the single-crystal X-ray diffraction (SCXRD) structure was studied to authenticate its solid-state structure. The as-synthesized MOF exhibited remarkable adsorption capacity towards various organic dyes, including Congo red (CR), rhodamine B (RhB), and methyl violet (MV), due to its ample surface area and strong π-π interactions between the pyrene moieties and dye molecules, as demonstrated by experimental and docking studies. The photocatalytic degradation of MV dye was also investigated. Detailed trapping tests indicate that hydroxyl (˙OH) and superoxide (O˙) radicals are likely the primary active species responsible for the photodegradation of the dye under study. Furthermore, the photocatalytic property of the MOF was investigated under visible light irradiation, demonstrating excellent ability to generate singlet oxygen. This study highlights the potential of pyrene-appended Zn(II)-based MOFs as promising materials for environmental remediation applications.