Metallophilic interactions in d(10)-d(10)(Au-I-Au-I)/d(8)-d(8)(Pt-II-Pt-II, Rh-I-Rh-I, Ir-I-Ir-I) complexes have been widely studied for decades, and metal metal (M M) bonding character has been revealed in both the ground and excited states. These M M closed-shell interactions are appealing driving forces for the self-assembly of supramolecular/polymeric systems, providing luminescent properties distinctly different from those of the corresponding monomer. However, reports on attractive interactions between two Au-III complex cations are scarce in the literature. Herein is described a series of pincer-type cationic Au-III complexes with different auxiliary ligands, among which the Au-III allenylidene complex displays a close Au-Au contact of 3.367 A between neighboring molecules in its X-ray crystal structure; Au-III-isocyanide complexes show a broad red-shifted absorption band and prominent phosphorescence upon aggregation that was influenced by an attractive Au-III-Au-III bonding interaction in the excited state; and Au-III-acetylene complexes can undergo living supramolecular polymerization upon varying the counteranion. The nature of the emissive excited state(s) of the Au-III aggregates is assigned to a mixture of major 3[pi-pi*] and minor (LMMCT)-L-3 (ligand-to-metal metal charge transfer) states based on combined spectroscopic and DFT/TDDFT studies. The morphology of the Au-III aggregates is highly dependent on the concentration and nature of the counteranion. A qualitative model has been applied to account for the concentration- and counteranion-dependent kinetics of the supramolecular polymerization process.