Li Guo

Hydrogels have great potential for application in tissue engineering and intelligent sensing fields due to their flexible, tough, and biocompatible characteristics. However, the limited mechanical properties of traditional hydrogels have severely hindered their practical applications. Inspired by the hierarchical anisotropic structure of natural biomaterials, this study proposes an effective structure‐molecule engineering strategy based on alignment/drying and salting out (ADSO) for constructing an anisotropic high‐amylose/polyvinyl alcohol (HSPI‐ADSO) hydrogel. This hydrogel exhibits a highly ordered hierarchical structure at the millimeter‐micrometer‐nanometer scale and a network structure at the nanometer‐molecular scale. The HSPI‐ADSO hydrogel demonstrates highly adjustable mechanical properties with the tensile strength of 4.18–17.40 MPa, the elongation at break of 258%–1086%, the Young's modulus of 3.33–37.43 MPa, and the toughness of 7.60–71.63 MJ·m ^{− 3} . Microscopic structure characterizations and finite element simulation confirm that this mechanism stems from the regulation of crystallinity, hydrogen bonds and the arrangement of the polymer chains by the ADSO strategy. Moreover, the ADSO strategy is also proven to have versatility to adjust the mechanical properties of other natural polymer‐based composite materials (alginate, konjac glucomannan and cellulose). Therefore, this method provides a highly promising idea for the application of these materials in tissue engineering, flexible electronics and biomedical materials fields.

BACKGROUND: With the implementation of plastic restriction policies and increasing environmental awareness, there is an urgent demand for starch‐based straws as alternatives to traditional plastic straws. In this study, three cationic polysaccharides, namely chitosan (CTS), chitosan oligosaccharide (COS), and cationic guar gum (CGG), were selected to prepare starch straws via thermoplastic extrusion. RESULTS: The results indicated that cationic polysaccharides enhanced the mechanical properties, hydrophobicity, compatibility, and short‐range order of the starch straws. Mechanistic analyses revealed the presence of hydrogen bonding and electrostatic interactions between starch and polysaccharides. Gaussian fitting indicated that the hydrogen bonding was dominated by OH⋯O. Among the samples, S‐COS exhibited the highest interaction energy (−58.94 kcal mol ⁻¹ ), complex index (598.3 g kg ⁻¹ ), and inter‐strand hydrogen bond energy (9.805 kcal mol ⁻¹ ). Consequently, S‐COS displayed the highest flexural strength, optimal flexural strain at break, and lower water absorption rate and swelling degree. S‐CGG demonstrated better flexibility and lowest water absorption. Additionally, after 150 days of storage, the surface of the starch–polysaccharide straws remained uniform without cracks. CONCLUSION: Our results demonstrated that starch–polysaccharide straws possessed excellent mechanical properties and water resistance, providing a theoretical basis for the development and industrial application of high‐performance starch‐based materials. © 2026 Society of Chemical Industry.