Octafunctionalized silsesquioxanes [(RsiO1.5)8, cubes] offer potential as rigid, hard nanoplatforms to which a variety of organofunctional groups can be appended. Crosslinking these groups leads to novel organic/inorganic nanocomposites that consist primarily of interfacial interactions. These materials can be 100% interphase. We present efforts to develop nanocomposite materials that consist of both continuous and discontinuous organic/inorganic phases. We then discuss methods of probing the properties of these materials.