Tough, Slippery, and Low-Permeability Multilayer Hydrogels Modified by Anisotropic Fiber Membrane for Soft Tissue Replacement

Hydrogels with sustained lubrication, high load-bearing capacity, and wear resistance are essential for applications in soft tissue replacements and soft material devices. Traditional tough or lubricious hydrogels fail to balance the lubrication and load-bearing functions. Inspired by the gradient-ordered multilayer structures of natural tissues (such as cartilage and ligaments), a tough, smooth, low-permeability, and low-friction anisotropic layered electrospun fiber membrane-reinforced hydrogel was developed using electrospinning and annealing recrystallization. This hydrogel features a stratified porous network structure of varying sizes with tightly bonded interfaces, achieving an interfacial bonding toughness of 1.6 × 103 J/m2. The anisotropic fiber membranes, mimicking the orderly fiber structures within soft tissues, significantly enhance the mechanical properties of the hydrogel with a fracture strength of 20.95 MPa, a Young’s modulus of 29.64 MPa, and a tear toughness of 37.94 kJ/m2 and reduce its permeability coefficient (6.1 × 10–17 m4 N–1 s–1). Meanwhile, the hydrogel demonstrates excellent solid–liquid phase load-bearing characteristics, which can markedly improve the tribological performance. Under a contact load of 4.1 MPa, the anisotropic fiber membrane-reinforced hydrogel achieves a friction coefficient of 0.036, a 219% reduction compared with pure hydrogels. Thus, the superior load-bearing and lubricating properties of this layered hydrogel underscore its potential applications in soft tissue replacements, medical implants, and other biomedical devices.