The latest advances in the area of polyoxometalate (POM)-based inorganic/organic hybrid materials prepared by self-assembly, covalent modification, and supramolecular interactions are presented. This Review is composed of five sections and documents the effect of organic cations on the formation of novel POMs, surfactant encapsulated POM-based hybrids, polymeric POM/organic hybrid materials, POMs-containing ionic crystals, and covalently functionalized POMs. In addition to their role in the charge-balancing, of anionic POMs, the crucial role of organic cations in the formation and functionalization of POM-based hybrid materials is discussed.
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