Cooking‐Inspired Versatile Design of an Ultrastrong and Tough Polysaccharide Hydrogel through Programmed Supramolecular Interactions

Abstract Simultaneously achieving strength and toughness in soft materials remains a challenge, especially for physically crosslinked hydrogels with many inactive interaction sites. In this work, inspired by the cooking of thick soup in China, a facile method that includes free water evaporation of the diluted pregel solution followed by crosslinking (WEC) is proposed to fabricate polysaccharide hydrogels. Herein, without the constraints of viscosity and crosslinking, polymer chains can homogenously approach as much as possible, thereby enabling the transformation of inactive supramolecular interaction (H‐bonding and ionic coordination) sites into active sites until reaching the maximum level. Through facilely tuning the concentrating degree, programmed supramolecular interactions, serving as energy‐dissipating sacrificial bonds, impart the hydrogels with strength and toughness over a very wide range, where a “ductile‐to‐tough” transition is discovered to occur first. Using WEC in alginate, the concentration can be as high as 25 wt% without sacrificing processing ability, a result that is significantly beyond common value (3–7 wt%), and the extremely stiff and tough hydrogels are obtained, superior to isotropic alginate hydrogels ever reported. This research offers a facile and versatile strategy to fabricate isotropic polysaccharide hydrogels, which become ideal matrix materials for further fabrication of hybrid or anisotropic hydrogels.