Hydrogels are flexible materials that have high potential for use in various applications due to their unique properties. However, their applications are greatly restricted by the low mechanical performance caused by high water content and inhomogeneous networks. This paper reports a universal strategy for easily preparing hydrogels that are tough and stretchable without any special structures or complicated processes. Our strategy involves tuning the polymerization conditions to form networks with many polymer chain entanglements to achieve energy dissipation. Tough and stretchable hydrogels can be prepared by free radical polymerization with a high monomer concentration and low cross-linker content to optimize the balance between physical and chemical cross-links by entanglements and covalent bonds, respectively. The strategy of using polymer chain entanglements for energy dissipation allows us to overcome the limitation of low mechanical performance, which leads to the wide practical use of hydrogels.

We designed biotin-conjugated four-armed poly(ethylene glycol) (biotinylated Tetra-PEG) as biomolecularly stimuli-responsive polymers that underwent the phase transition from a sol to a gel state in response to avidin as a target biomolecule.

Temperature-responsive poly(N-isopropylacrylamide) (PNIPAAm) gels were prepared via atom transfer radical polymerization (ATRP), and their mechanical and responsive properties were investigated from the viewpoint of their network homogeneity.

The network structures of poly(N-isopropylacrylamide) (PNIPAAm) gels prepared by atom transfer radical polymerization (ATRP) were compared with those prepared by free radical polymerization (FRP), as a conventional radical polymerization. Temperature-responsive...