Light‐Triggered In Situ Gelation of Hydrogels using 2D Molybdenum Disulfide (MoS2) Nanoassemblies as Crosslink Epicenter

Abstract Light‐responsive biomaterials are an emerging class of materials used for developing noninvasive, noncontact, precise, and controllable biomedical devices. Long‐wavelength near‐infrared (NIR) radiation is an attractive light source for in situ gelation due to its higher penetration depth and minimum side effects. The conventional approach to obtain crosslinked biomaterials relies heavily on the use of a photoinitiator by generating reactive species when exposed to short‐wavelength radiation, which is detrimental to surrounding cells and tissue. Here, a new class of NIR‐triggered in situ gelation system based on defect‐rich 2D molybdenum disulfide (MoS 2 ) nanoassemblies and thiol‐functionalized thermoresponsive polymer in the absence of a photoinitiator is introduced. Exposure to NIR radiation activates the dynamic polymer–nanomaterials interactions by leveraging the photothermal characteristics of MoS 2 and intrinsic phase transition ability of the thermoresponsive polymer. Specifically, upon NIR exposure, MoS 2 acts as a crosslink epicenter by connecting with multiple polymeric chains via defect‐driven click chemistry. As a proof‐of‐concept, the utility of NIR‐triggered in situ gelation is demonstrated in vitro and in vivo. Additionally, the crosslinked gel exhibits the potential for NIR light‐responsive release of encapsulated therapeutics. These light‐responsive biomaterials have strong potential for a range of biomedical applications, including artificial muscle, smart actuators, 3D/4D printing, regenerative medicine, and therapeutic delivery.