Ultra‐High Modulus Hydrogels Mimicking Cartilage of the Human Body

The human body is comprised of numerous types of cartilage with a range of high moduli, despite their high hydration. Owing to the limitations of cartilage tissue healing and biological grafting procedures, synthetic replacements have emerged but are limited by poorly matched moduli. While conventional hydrogels can achieve similar hydration to cartilage tissues, their moduli are substantially inferior. Herein, triple network (TN) hydrogels are prepared to synergistically leverage intra‐network electrostatic repulsive and hydrophobic interactions, as well as inter‐network electrostatic attractive interactions. They are comprised of an anionic 1st network, a neutral 2nd network (capable of hydrophobic associations), and a cationic 3rd network. Collectively, these interactions act synergistically as effective, yet dynamic crosslinks. By tuning the concentration of the cationic 3rd network, these TN hydrogels achieve high moduli of ≈1.5 to ≈3.5 MPa without diminishing cartilage‐like water contents (≈80%), strengths, or toughness values. This unprecedented combination of properties poises these TN hydrogels as cartilage substitutes in applications spanning articulating joints, intervertebral discs (IVDs), trachea, and temporomandibular joint disc (TMJ). Triple network hydrogels, leveraging electrostatic and hydrophobic interactions, are developed as potential substitutes for various cartilage tissues found in the human body. These hydrogels achieve moduli (i.e., stiffnesses) that parallel several cartilage types, and are also hydrated, strong, and tough. Thus, these hydrogels are promising candidates as cartilage substitutes in numerous applications.