New types of polymer hydrogels (nanocomposite gels, NC gels) and soft polymer nanocomposites (M-NCs) with novel organic/inorganic network structures were synthesized using disk-like inorganic clay nanoparticles as multifunctional crosslinkers to form new network systems. Both NC gels and M-NCs have extraordinary optical and mechanical properties, such as ultrahigh reversible extensibility, as well as a number of new characteristics relating to polymer/clay morphology, stimulus-sensitivity, biocompatibility, surface properties, micropatterning and so on. The serious disadvantages (intractability, mechanical fragility, optical turbidity, poor processing ability, low stimulus sensitivity) associated with the conventional, chemically crosslinked polymeric materials were overcome in NC gels and M-NCs.