biostudies-literatureLiu ZQingLan Project of Jiangsu ProvinceHigh-end Talent Project of Yangzhou UniversityPriority Academic Program Development of Jiangsu Higher Education InstitutionsNational Natural Science Foundation of ChinaKey Research and Development Plan of Shaanxi ProvinceChinese Aeronautical Establishment Aeronautical Science FoundationNatural Science Foundation of Jiangsu Provincee04778https://www.ebi.ac.uk/biostudies/studies/S-EPMC12376593biostudies-literatureUnknown12(30)Anisotropic hydrogels are promising candidates as load-bearing materials for tissue engineering, while huge challenges remain in exploring effective and scalable methods for the preparation of anisotropic hydrogels with simultaneous high tensile strength, large toughness, good fracture strain, excellent fatigue and swelling resistances. Inspired by the brick-and-mortar layered structure of nacre and the hierarchical fibril strucure of soft tissues (e.g., tendon and ligament), a facile organogel-assissted calendering strategy is reported to design anisotropic hydrogels with a highly oriented and dense fiber lamellar strucure. The synergy of shearing and annealing promotes macromolecular chain alignment and crystallinity along the calendering direction while forming a nacre-like lamellar morphology in the thickness direction. The tensile strength, elastic modulus, toughness and fracture energy of the anisotropic hydrogels can reach as high as 41.0 ± 6.4 MPa, 67.0 ± 5.1 MPa, 46.2 ± 3.3 MJ m^-3, and 62.20 ± 8.55 kJ m^-2, respectively. More importantly, the hydrogels show excellent crack growth and swelling resistances with the fatigue threshold increased to 2170 J m^-2. This study provides a promising approach for fabrication of large-sized biomimetic anisotropic hydrogels with outstanding mechanical properties for biomedical and engineering applications.Advanced science (Weinheim, Baden-Wurttemberg, Germany)Highly Oriented Bio-Mimetic Hydrogels by Calendering.PMC1237659352473049BK20240934124723922023-GHZD-122023004105300612272307Li HZhang DMai YWGu WGao JWang GWu HShi YLiu ZTang LSong PHuang XMiao YWang YXie AYin JfalseHighly Oriented Bio-Mimetic Hydrogels by Calendering.Anisotropic hydrogels are promising candidates as load-bearing materials for tissue engineering, while huge challenges remain in exploring effective and scalable methods for the preparation of anisotropic hydrogels with simultaneous high tensile strength, large toughness, good fracture strain, excellent fatigue and swelling resistances. Inspired by the brick-and-mortar layered structure of nacre and the hierarchical fibril strucure of soft tissues (e.g., tendon and ligament), a facile organogel-assissted calendering strategy is reported to design anisotropic hydrogels with a highly oriented and dense fiber lamellar strucure. The synergy of shearing and annealing promotes macromolecular chain alignment and crystallinity along the calendering direction while forming a nacre-like lamellar morphology in the thickness direction. The tensile strength, elastic modulus, toughness and fracture energy of the anisotropic hydrogels can reach as high as 41.0 ± 6.4 MPa, 67.0 ± 5.1 MPa, 46.2 ± 3.3 MJ m^-3, and 62.20 ± 8.55 kJ m^-2, respectively. More importantly, the hydrogels show excellent crack growth and swelling resistances with the fatigue threshold increased to 2170 J m^-2. This study provides a promising approach for fabrication of large-sized biomimetic anisotropic hydrogels with outstanding mechanical properties for biomedical and engineering applications.2025-01-01T00:00:00Z2025 Aug2026-05-09T17:46:37.221Z2026-04-08T01:07:05.287ZS-EPMC123765934053613310.1002/advs.202504778