The major organic component in carbonaceous chondrites is a highly aromatic macromolecular material. Aromatic organic matter and phyllosilicates are colocated in these meteorites, and it is possible that the physical association represents a synthetic chemical relationship. To explore the potential reactions that could take place to produce the aromatic macromolecular material, we heated various simple aromatic units in the presence of montmorillonite with different exchanged cations. The majority of cation-exchanged montmorillonites tested, sodium-, aluminum-, iron-, nickel-, and cobalt-rich montmorillonites, do not produce polymerization products. By contrast, Fe(3+) cation-exchanged montmorillonite readily facilitates addition reactions between aromatic hydrocarbons. A feasible mechanism for the process is oxidative coupling, which involves a corresponding reduction of the Fe(3+) cation to its Fe(2+) counterpart. A similar reduction process for the other metal cations does not take place, highlighting the importance of iron. This simple process is one feasible mechanism for the construction of aromatic macromolecules such as those found in carbonaceous chondrites. The search for a relationship between Fe(3+)-rich phyllosilicates and aromatic organic structures (particularly dimers, trimers, and more polymerized forms) in carbonaceous chondrites would represent an effective test for constraining the role of clay catalysis in the early Solar System.