A series of high clay content Laponite XLS/polyacrylamide (PAAm) nanocomposite hydrogels (S-M gels) with excellent resilience, low elastic hysteresis, and ultrahigh elongation, have been successfully synthesized. Based on our results, it is concluded that the mechanical properties of nanocomposite hydrogels probably depend to a great extent on the hydrophilicity and flexibility of the macromolecules. Moreover, it is found that the transparency during the in-situ polymerization of S-M gels does not change, which is quite different from clay/poly(N-isopropylacrylamide) nanocomposite hydrogels.