Single-crystal X-ray diffraction studies have confirmed that Ni3S3-based molecular bowls prepared in one-pot reactions capture either CH2Cl2 or C-60. The nature of the pendant substituents (naphthalen-2-ylmethyl, benzyl, or ethyl) around the rim of the bowl dictates the formation of a 1:1 (bowl host-C-60 guest) or 2:1 (capsule host-C-60 guest) architecture. In CDCl3, the trimeric complexes were found to be in equilibrium with dimeric analogues. For the naphthalen-2-ylmethyl-substituted host, NMR spectroscopic titration data confirmed a 1:1 host-C-60 guest complex in 1,2-Cl2C6D4 solution.