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Hydrogels with adhesive properties have potential for numerous biomedical applications. Here, the design of a novel, intrinsically adhesive hydrogel and its use in developing internal therapeutic bandages is reported. The design involves incorporation of “triple hydrogen bonding clusters” (THBCs) as side groups into the hydrogel matrix. The THBC through a unique “load sharing” effect and an increase in bond density results in strong adhesions of the hydrogel to a range of surfaces, including glass, plastic, wood, poly(tetrafluoroethylene) (PTFE), stainless steel, and biological tissues, even without any chemical reaction. Using the adhesive hydrogel, tissue‐adhesive bandages are developed for either targeted and sustained release of chemotherapeutic nanodrug for liver cancer treatment, or anchored delivery of pancreatic islets for a potential type 1 diabetes (T1D) cell replacement therapy. Stable adhesion of the bandage inside the body enables almost complete tumor suppression in an orthotopic liver cancer mouse model and ≈1 month diabetes correction in chemically induced diabetic mice.

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Hydrogels are used in a variety of applications ranging from tissue engineering to soft robotics. They often undergo large deformation coupled with solvent diffusion, and structural integrity is important when they are used as structural components. This paper presents a thermodynamically consistent method for calculating the transient energy release rate for crack growth in hydrogels based on a modified path-independent J-integral. The transient energy release rate takes into account the effect of solvent diffusion, separating the energy lost in diffusion from the energy available to drive crack growth. Numerical simulations are performed using a nonlinear transient finite element method for center-cracked hydrogel specimens, subject to remote tension under generalized plane strain conditions. The hydrogel specimen is assumed to be either immersed in a solvent or not immersed by imposing different chemical boundary conditions. Sharp crack and rounded notch models are used for small and large far-field strains, respectively. Comparisons to linear elastic fracture mechanics (LEFM) are presented for the crack-tip fields and crack opening profiles in the instantaneous and equilibrium limits. It is found that the stress singularity at the crack tip depends on both the far-field strain and the local solvent diffusion, and the latter evolves with time and depends on the chemical boundary conditions. The transient energy release rate is predicted as a function of time for the two types of boundary conditions with distinct behaviors due to solvent diffusion. Possible scenarios of delayed fracture are discussed based on evolution of the transient energy release rate.