C-60 subset of[Cu26Cl26L2{Cp*Fe(P-eta 5-(5))}(13)(CH3CN)(9)] (L = H2O) represents a first example of a complete encapsulation of C-60 itself by an inorganic fullerene-like system via molecular recognition of the five- and sixfold-symmetric structural motif of C-60. The product exhibits an inorganic cover consisting of 99 inorganic core atoms from pentaphosphaferrocene and Cu(I) chloride building blocks. This is the first instance of a hollow structure that completely encapsulates C-60. The overall spherical molecule possesses an outer diameter of 2.3 nm and shows a remarkable electronic interaction between C-60 and the encapsulating giant molecule.