Polysilsesquioxanes are regarded as organic–inorganic hybrid materials at a molecular level. We can readily tune the properties of the materials for realizing the desired ones by changing the contents or types of organic components. In addition, the hierarchical structures have potential for generating further characteristics distinctly different from those of the constituents. From this viewpoint, polyhedral oligomeric silsesquioxane (POSS) is attractive as a cornerstone in highly ordered materials. In this review, we survey recent studies on modified POSS-based functional materials and particularly explain the design concepts for applying the significant characteristics of POSS for the material properties. In the initial sections, we introduce the examples concerning intrinsic properties of POSS such as thermal stability, mechanical property, and structural features. In the latter sections, we describe the application of POSS-based materials for bio-relating functional materials. We describe the validity of POSS for molecular designing of the advanced imaging tools.
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