A novel type of polymer nanocomposite (NC) hydrogel with extraordinary mechanical properties at low inorganic content is prepared and investigated. The NC hydrogels consist of isethionate-loaded layered double hydroxide/polyacrylamide (LDH-Ise/PAM) - with LDH-Ise being used because of its swelling properties and no conventional organic crosslinker. The NC hydrogels exhibit an unusual hierarchical porous structure at the micro- and nanometer scales, and their elongation at break can exceed 4000%.