Single crystals of three-dimensional (3D) C60 polymer were prepared by the topotactic conversion of two-dimensional (2D) C60 polymer single crystals at a pressure of 15 GPa at 600°C. The x-ray single crystal study revealed that the 3D C60 polymer crystallized in a body centered orthorhombic space group Immm, and spherical C60 monomer units were substantially deformed to rectangular parallelepiped (cuboidal) shapes, each unit being bonded to eight cuboidal C60 neighbors via [3+3] cycloaddition. The 3D C60 polymer was electron conductive, in contrast with the nonconductive behavior of 2D polymers.