We report a facile approach to fabricate an Ag-embedded fullerene (C-60) catalyst by the chemical reduction of the AgNO3 complex encapsulated fullerene microcrystal, which showed an enhanced catalytic reduction of 4-nitrophenol because of the strong absorption and propagation of H-2 along the fullerene surface. With the aid of visible-light radiation, photodegradation of orange G dye is achieved through the formation of an electron donor-acceptor dyad between plasmon Ag nanostructures and fullerene molecules, which effectively offsets the "electron-hole" recombination. Neither Ag nanoparticle nor fullerene crystal used in isolation could perform this chemical conversion, implying that the metal-fullerene hybrid structure is imperative for performing the catalytic reaction. The obtained Ag-embedded fullerene crystal is characterized by scanning electron microscopy (SEM), associated energy-dispersive X-ray spectroscopy (EDX) imaging, and X-ray photoelectron spectroscopy (XPS) and demonstrates that the present hybrid materials would add a supplemental member to a family of photocatalysts toward the organic synthesis and wastewater remediation.