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Novel double-network (DN) hydrogels with high mechanical strength have been fabricated with two biocompatible polymers, poly(vinyl alcohol) (PVA) and poly(ethylene glycol) (PEG), through a simple freezing and thawing method. Some properties of the obtained hydrogels, such as the mechanical strength, rheological and thermodynamic behavior, drug release, and morphology, have been characterized. The results reveal that in sharp contrast to most common hydrogels made with simple natural or synthetic polymers, PVA/PEG hydrogels can sustain a compressive pressure as high as several megapascals, highlighting their potential application as biomedical materials. In addition, a model for describing the structural formation of PVA/PEG DN hydrogels is proposed: the condensed PVA-rich phase forms microcrystals first, which bridge with one another to form a rigid and inhomogeneous net backbone to support the shape of the hydrogel, and then the dilute PEG-rich phase partially crystallizes among the cavities or voids of the backbone; meanwhile, there are entanglements of molecular chains between the two polymers. Moreover, a mechanism is also proposed to explain the high mechanical strength of PVA/ PEG DN hydrogels. It is suggested that the free motion of PEG clusters in the cavities of PVA networks can prevent the crack from growing to a macroscopic level because the linear PEG chains in the cavities effectively absorb the crack energy and relax the local stress either by viscous dissipation or by large deformation of the PEG chains.

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