Nine new double-salt compounds have been prepared and six crystal structures are reported that demonstrate a general metathesis route to double-salt compounds with metallophilic interactions. The compounds contain [ Pt( terpy) X](+) or [ Au( bpy) X-2](+) cations, Au-III or Au-I anions such as [ AuBr4](-) or [ AuCl2](-), and are prepared in water and recrystallized from organic solvents. In all crystallographically characterized cases, there exist metallophilic interactions between cations and anions, demonstrating the power of this general route. In most cases, there exists an unbroken chain of metallophilic interactions through the crystal, forming single-atom-wide wires.