Despite the early promise of phototunable gels, chemistry-and material-based limitations have precluded the full power of these platforms from being realized . Reliance on organic chromophores to encode photodegradability within hydrogels has historically confined the photocleaving wavelengths to high-energy light -ranging from £365 nm for ortho-nitrobenzyl (oNB)-based systems up to 450 nm for some reported photolabile coumarins and bimanes . While some of these chromophores have been highly characterized and are cytocompatible throughout photolysis, the utilization of UV light irradiation has traditionally confined these materials to solely in vitro use as high-energy light is poorly penetrant through complex tissue . Additionally, only a limited number of reports have described materials that are sensitive to multiple orthogonal wavelengths, of which nearly all crosslinkers employed rely heavily on near-and far-UV light , thereby missing significant opportunities for cytocompatible material multiplexing by taking advantage of the entire spectrum of visible and IR light. A collection of photocleavable crosslinkers that distinctly responds to an expanded portion of electromagnetic spectrum, enabling deeper tissue penetration and multiplexed wavelength-selective material modulation using differently colored light, would enable exciting new directions for phototunable hydrogel platforms.