A new method to synthesize fullerene and sulfur compounds has been developed. Using this method, C60S16 and C70S16 compounds were grown from dilute fullerene and sulfur toluene solution. Their atomic structures were analyzed by x-ray diffraction with the single crystal. The C60S16 crystal is C-centered monoclinic structure of a = 2.0874 nm, b = 2.1139 nm, c = 1.05690 nm and β = 111.93°, and the C70S16 has a primitive monoclinic, P21/c, with lattice parameters of a=1.5271 nm, b=1.49971 nm, c=2.18024 nm and β=109.791°. In this compound, the structure of fullerenes is maintained and sulfur atoms form S8 rings placed around the fullerenes.