It is shown that C-60 Single crystals can be polymerized under relativ
ely modest pressure-temperature conditions. The resulting single cryst
als exhibit long-range order and they are made up of 12 orientation va
riants. The structure is orthorhombic with a short intermolecular dist
ance along the chains (9.14 Angstrom), characteristic of covalent bond
ing. We propose a structural mechanism for the polymerization of fulle
rene-based compounds; it involves a shift of one of the (111) cubic pl
anes together with a shortening of the (111) spacing. The configuratio
n of the polymer chains presents interesting relations with that found
in the A(1)C(60) polymer compounds.