he obtained results indicate that watersoluble cyclodextrin–fullerene complexes show unique photophysical and biological properties. Recently, our studies indicated that the resultant complexes of bis-cyclodextrins and pharmacy molecules significantly enhance both water solubility and biological activity of fullerene derivatives.[21] Herein, we report a simple way to prepare a water-soluble fullerene assembly with a coordinated metal center through end-to-end intermolecular inclusion complexation of a dimeric cyclodextrin with a fullerene. Furthermore, the assembly behavior of this complex has been comprehensively investigated by UV/Vis absorption, FTIR, 1H NMR, and 13C NMR spectroscopies, elemental analysis, thermogravimetric analysis (TGA), scanning tunneling microscopy (STM), transmission electron microscopy (TEM), and scanning electron microscopy (SEM). The biological activity of the assembly was assayed under visible light irradiation and another in dark as a control, which indicates that the assembly may serve as an effective photodriven DNA cleaver.