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Biomedical materials are advancing in their complexity to meet the widespread needs of a range of clinical scenarios, including towards applications in tissue engineering and the delivery of therapeutics (e.g., cells, drugs) (1). Biomaterials have evolved from relatively static systems, to those that undergo degradation via hydrolysis or enzymatic erosion, and more recently to materials with dynamic properties. This evolution in material design has been particularly useful in the delivery of therapeutic molecules, where the ability to temporally refine and control the release of a payload is both desirable and necessary. Stimuli-responsive materials are evolving as ‘smart’ delivery systems where the release of encapsulated molecules is controlled through external triggers, which may be in response to the physiological environment (e.g., enzymes) (2,3) or through sensitivity to an externally applied stimulus (4-9). In the cases of material systems where an external cue is desired, triggers including ultrasound (10), light (4,6,9) and magnetic fields (7,8) have enabled noninvasive modulation of therapeutic payload delivery. In particular, light offers an accessible trigger with high spatiotemporal control, and near-infrared (NIR) light is especially attractive due to its minimal absorbance in vivo when compared with shorter wavelengths (11,12). This allows for greater depth penetration and is one reason why NIR light is currently employed in clinical practice (e.g., medical imaging) (13). Recent studies have explored NIR and light attenuation when used in vivo (14). NIR photons can interact with photosensitive molecules and particles to trigger photochemical reactions (9) or to generate heat by the photothermal effect (4,15-18). Thus, the inclusion of gold nanoparticles (e.g., gold nanorods or AuNRs), which interact with NIR light, in materials allows plasmonic heating in response to NIR illumination. This enables AuNRs to be combined with stimuli-responsive (19) polymeric systems that possess temperature-dependent properties (20-22) (e.g., lower critical solution temperature, glass transition temperature) for light-sensitive release of encapsulated therapeutics. Here, AuNRs were combined with hydrogels crosslinked by stimuli responsive, supramolecular bonds between β-cyclodextrin (CD) and adamantane (Ad). CD and Ad form host-guest inclusion complexes that are stabilized primarily by hydrophobic interactions and this interaction is reversible. This supramolecular interaction can be disrupted by shear forces, by competing hydrophobic interactions, or by energy that increases molecular motion (e.g., heating). The ability to undergo shear-thinning permits the injectability...