Abstract: Using the zirconium-based metal-organic framework UiO-66 as the structural platform, NH₂-UiO-66 was constructed by ligand amination, and its catalytic applicability in dye-sensitized solar cells (DSSCs) and alkaline hydrogen evolution reaction (HER) was evaluated. The structural and morphological characterization of the synthesized materials was conducted using X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), Raman spectroscopy (Raman), and nitrogen adsorption-desorption curves (BET). The results showed that the material framework structure remained stable, the morphology was uniform, and it had a high specific surface area and pore characteristics, providing a structural basis for electrolyte infiltration and reactant mass transfer; X-ray photoelectron spectroscopy (XPS) and infrared spectroscopy (FTIR) further confirmed the successful introduction of amino functional groups and the modulation of the surface chemical environment. Based on the synergistic effect achieved through the amino modification strategy, the NH₂-UiO-66 catalyst exhibited a low overpotential of 105 mV and a Tafel slope of 92 mV·dec⁻¹ in HER (1.0 mol/L KOH). When NH₂-UiO-66 was used as the counter electrode in DSSC, a 7.95% power conversion efficiency was achieved in the N719-I₃⁻/I⁻ electrolyte system, significantly superior to UiO-66 (6.98%) and Pt (7.30%) electrodes. This study provides a new idea for constructing multifunctional non-noble-based electrocatalytic counter electrode materials by regulating MOF functional groups.