(A) Internal components of a casein-reinforced polyacrylamide (PAM) hydrogel, and (B) schematic illustration of the toughening mechanism of casein additives due to energy dissipation through hydrophobic interactions. (C) The tensile mechanical properties, and (D) transmission electron microscopy (TEM) images of casein micelles in the hydrogels (reprinted with permission from ref 94). (E) Fabrication process of tough nanocomposites mediated by incorporating calcium hydroxide (Ca(OH)2) nano-spherulites (CNS) in a PAM network. The Ca3SiO5 releases Ca2+ and OH- in a hydration process during which the small-sized CNS particles (<5 nm in size) are crystallized at 0 °C. The persulfate ions from the ammonium persulfate (APS) initiator are attracted electrostatically to CNS and act as crosslinkers. (F) Significant improvement of stretchability in PAM networks with small amounts of CNS. Reprinted by permission from ref 96. Nature Publishing Group, Copyright 2016. (G) Fabrication steps of montmorillonite (MMT)/PAM composite hydrogels. (H) Digital photographs of bow-tied hydrogel, and tensile stretching of the hydrogels over 12000%. Reprinted with permission from ref 99. Copyright 2015 American Chemical Society. (I) Preparation of vinyl functionalized hybrid silica nanoparticles (VSNPs)-poly(acrylic acid) (PAA) hydrogels where VSNP nanoparticles act as crosslinking points. (J) The mechanism explaining the improved hydrogel stretchability and molecular mechanism of deformation. (K) Stress-strain characteristics of the hydrogels with different amounts of VSNP nanoparticles, and (L) illustration of manually stretched hydrogels. Reprinted by permission from ref 107. Nature Publishing Group, Copyright 2015.