Introduction and Overview. Synthesis of Viologens. Spectroscopic Properties of Viologen Species. The Structure of Bipyridilium Species. The Dication: Charge-transfer Equilibria. The Radical Cation: Dimer Formation. The Di-Reduced Bipyridilium Species: The Comproportionation Reaction. Adsorption of the Viologens. Electrochemistry and Electron-transfer Reactions. Photochemistry of the Viologens and Solar-energy Conversion. Electron Mediation, Herbicidal Activity and Toxicity. Electrochromism in Viologen-based Systems. Solid-state Conductivity and use of Viologens in Molecular Electronics. Supramolecular and Self Assembly Chemistry of the Viologens. Indexes.