Current research efforts focus on using metal ions to bring organic molecules together and in so doing form structures that resemble large common materials, such as boxes, cages, grids, and channels. These metal-organic supramolecular structures are at the interface between molecular and macromolecular chemistry. As a contribution to this field of chemistry, we have focused on binding metal ions to cupped-shaped template molecules, which can be appended with functional groups. These resorcinarene-based molecules have four phenyl groups linked together into a ring and various functional groups attached to their upper rim. Some of the functional groups, bispyridylmethylamine (bpa) and iminodiacetic acid, are able to coordinate to metal ions. In the case of the bispyridylmethylamine resorcinarene, 2, a tetranuclear metal complex is formed when it is allowed to coordinate to copper(II). The copper centers surround the resorcinarene cavity and are not electronically coupled. In contrast to the Cu₄2⁸⁺ complex, when cobalt(II) or iron(II) are allowed to coordinate to an iminodiacetic acid resorcinarene, 3, two resorcinarenes are bought together. The M₄3₂^8- (M = Co or Fe) complexes are tetranuclear metal(II) cage compounds that assemble in aqueous solutions above pH 4 and have a cavity. These molecules are capable of encapsulating a variety of organic guest molecules, for example, nonpolar hydrocarbons, substituted phenyls, alcohols, halogen containing hydrocarbons, and polar organic molecules. The cages act as NMR shift reagents and cause substantial up-field isotropic hydrogen shifts (-30 to -40 ppm for Co²⁺ and -5 to -15 ppm for Fe²⁺) in the guest molecule and separation of the guest hydrogen chemical shifts. The solid state structures of Ba₄[M₄³₂guest] (guest = 6 H₂O, bromobenzene, or ethylbenzene) show bond angles independent of whether the metal ion is cobalt or iron, and bond lengths typical of metal oxygen and nitrogen bonds. The encapsulated guest does not noticeably effect the cavity dimensions, bond lengths, and bond angles.