A new approach for the construction of functionalized metallosupramolecular tetragonal prisms via multicomponent, coordination-driven, template-free self-assembly is described. The combination of tetra-(4-pyridylphenyl)ethylene, a 90 degrees Pt(II) acceptor, and ditopic bipyridine or carboxylate ligands functionalized with hydroxyl or amine groups, hydrophobic alkyl chains, or electrochemically active ferrocene, yields a suite of seven self-assembled tetragonal prisms under mild conditions. These three-dimensional metallosupramolecules were characterized by multinuclear NMR (P-31 and H-1) and mass spectrometry. Their shapes and sizes were established using Merck Molecular Force Field (MMFF) simulations. In addition, their approximate sizes were further supported by pulsed-field-gradient spin echo (PGSE) NMR experiments.