Mechanically Robust Lubricating Hydrogels Beyond the Natural Cartilage as Compliant Artificial Joint Coating

Abstract Natural cartilage exhibits superior lubricity as well as an ultra‐long service lifetime, which is related to its surface hydration, load‐bearing, and deformation recovery feature. Until now, it is of great challenge to develop reliable cartilage lubricating materials or coatings with persistent robustness. Inspired by the unique biochemical structure and mechanics of natural cartilage, the study reports a novel cartilage‐hydrogel composed of top composite lubrication layer and bottom mechanical load‐bearing layer, by covalently manufacturing thick polyelectrolyte brush phase through sub‐surface of tough hydrogel matrix with multi‐level crystallization phase. Due to multiple network dissipation mechanisms of matrix, this hydrogel can achieve a high compression modulus of 11.8 MPa, a reversible creep recovery (creep strain: ≈2%), along with excellent anti‐swelling feature in physiological medium (v/v 0 < 5%). Using low‐viscosity PBS as lubricant, this hydrogel demonstrates persistent lubricity (average COF: ≈0.027) under a high contact pressure of 2.06 MPa with encountering 100k reciprocating sliding cycles, negligible wear and a deformation recovery of collapse pit in testing area. The extraordinary lubrication performance of this hydrogel is comparable to but beyond the natural animal cartilage, and can be used as compliant coating for implantable articular material of UHMWPE to present, offering more robust lubricity than current commercial system.