Fabrication of hydrogels with unique microstructures and better mechanical properties through the self-assembly of commercially available synthetic polymers and small molecules is of great scientific and practical importance. A type of physical hydrogels is prepared by the self-assembly of polyvinyl alcohol (PVA) and tannic acid (TA) in aqueous solution with a low PVA–TA concentration (0.5–6.0 wt %) at room temperature. With the increase of the PVA–TA concentration, the water content of the hydrogels increases, and the content of TA in the hydrogels decreases from 23.1 to 6.4%. The driving force for the self-assembly is proven to be the hydrogen bonding between PVA and TA, which also induces the crystallization of PVA chains. The self-assembled PVA–TA hydrogels have diverse morphologies that change from microspheres to oriented porous structures with the increase of the PVA–TA concentration, and these structures are all composed of nanosized particles, fibers, and/or sheets. Most of the self-assembled PVA–TA hydrogels show good mechanicalproperties. The highest tensile strength and elastic modulus of thePVA–TA hydrogel prepared with 1.0 wt % PVA–TA concentrationare about 84 and 30 kPa, respectively. This self-assembly method wouldlead to the fabrication of more hydrogels with unique microstructuresand properties for practical applications.
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