The invention provides injectable, tough hydrogels that can be crosslinked in situ
on demand using minimally-invasive methods, such as visible
light exposure is an unmet medical challenge. Among the emerging biopolymers for tissue sealing,
gelatin methacryloyl (GelMA), a naturally-derived
biopolymer obtained from denatured collagen, has secured a promising role as a result of its excellent bioadhesion,
biodegradation, and
biocompatibility. To overcome one of the main shortcomings of GelMA, i.e.,
brittleness, we hybridized it using
methacrylate-modified alginate (AlgMA) to impart
ion-induced reversible crosslinking that can dissipate energy under strain. The
hybrid GelMA-AlgMA hydrogels provide a photocrosslinkable, injectable, and
adhesive platform with an excellent
toughness that can be engineered using
divalent cations, such as
calcium. This class of novel
hybrid biopolymers with more than 600% improved
toughness may set the stage for durable, mechanically-resilient, and cost-effective tissue sealants in minimally
invasive procedure, especially for stretchable tissues.