We have fabricated new types of polymer hydrogels and polymer nanocomposites, that is, nanocomposite gels (NC gels) and soft polymer nanocomposites (M-NCs), with novel organic/inorganic network structures. Both NC gels and M-NCs were synthesized by in situ free-radical polymerization in the presence of exfoliated clay platelets in aqueous systems and were obtained in various forms and sizes with a wide range of clay contents. Here, disk-like inorganic clay nanoparticles function as multifunctional crosslinkers to form new types of network systems. NC gels have extraordinary optical, mechanical and swelling/deswelling properties, as well as a number of new characteristics relating to optical anisotropy, polymer/clay morphology, biocompatibility, stimuli-sensitive surfaces, micropatterning and so on. The M-NCs also exhibit dramatic improvements in optical and mechanical properties including ultrahigh reversible extensibility and well-defined yielding behavior, despite their high clay contents. Thus, the serious disadvantages (intractability, mechanical fragility, optical turbidity, poor processing ability, low stimulus sensitivity and so on) associated with the conventional, chemically crosslinked polymeric materials were overcome in NC gels and M-NCs. Polymer Journal (2011) 43, 223-241; doi: 10.1038/pj.2010.141; published online 19 January 2011