Herein, we have fabricated starch–borax double cross-linked network (DC) hydrogels with tough and self-healing properties using a one-pot method. The addition of borax significantly increased the storage modulus and loss modulus of these starch–borax DC hydrogels. The maximum compression stress (~288 kPa) of starch–borax DC hydrogels containing 5% borax was about ten times greater than that of a pure-starch hydrogel. The texture profile analysis values of the DC hydrogels—including hardness, springiness, cohesiveness, and adhesiveness—increased compared to pure-starch hydrogels. In addition, starch–borax DC hydrogels exhibited excellent self-healing and shape-recovery properties. These DC hydrogels, with a variety of excellent properties, have potential applications in agricultural, biomedical, and industrial fields.

The aim of this study was to employ molecular dynamics simulations to elucidate the mechanism involved in amylose–zein complexation and the stability of the molecular conformation of amylose–zein complexes in water at the atomic and molecular levels. The average root mean square deviation and radius of gyration were lower for amylose–zein complexes (1.11 nm and 1 nm, respectively) than for amylose (2.13 nm and 1.2 nm, respectively), suggesting a significantly higher conformational stability for amylose–zein complexes than for amylose in water. The results of radial distribution function, solvent-accessible surface area, and intramolecular and intermolecular hydrogen bonds revealed that the amylose–zein interaction inhibited water permeation into the amylose cavity, leading to enhanced conformational stabilities of the V-type helical structure of amylose and the amylose–zein complexes. Furthermore, the amylose in amylose–zein complexes displayed the thermodynamically stable ⁴C₁ conformation. These findings can provide theoretical guidance in terms of the application of protein on starch processing aiming to improve the physicochemical and functional properties of starch (such as swelling capacity, pasting properties, and digestibility) for developing novel low-digestibility starch–protein products.