Metal positions in endohedral metallofullerenes (EMFs) are of special importance because their molecular symmetry and intrinsic properties are strongly influenced by the location and motion of the encapsulated metals. X-ray analyses of the cocrystals of Gd@C-2v(9)-C-82 with nickel(II) octaethylporphyrin [Ni-II(OEP)] reveal that the Gd3+ cation is off-center, being located under a hexagonal ring along the 2-fold axis of the C-2v(9)-C-82 cage. This result is in sharp contrast to that of a previous study, showing that Gd@C-2v(9)-C-82 has an anomalous endohedral structure, with the metal being positioned over a [6,6] bond, which is opposite to the hexagonal ring along the C-2 axis (Phys. Rev. B 2004, 69, 113412). In agreement with theoretical calculations and related studies, it is conclusive that the single rare-earth metal in M@C-2v(9)-C-82 always tends to coordinate with the hexagonal ring along the 2-fold axis, instead of interacting with the [6,6] bond on the other end, regardless of the type of metal atom.