In this work, we describe the synthesis and properties of a new series of photolabile crosslinkers, including two based on novel ruthenium compounds: (1) Ru(2,2'-biquinoline)2(4azidobutanenitrile)2 (denoted Rubiq); (2) (Ru(2,2'-bipyridine)2(4-azidobutanenitrile)2 (Rubpy); and (3) an established oNB with wavelength-separated lmax capable of respectively responding selectively to three different colors of visible light -red (617 nm), green (530 nm), and blue (405 nm) (Fig. ). Mixing four-arm poly(ethylene glycol) (PEG) end-functionalized with bicyclononyne (PEG-tetraBCN) together with the bis(azide)-modified photolinkers with 1:1 stoichiometry with respect to their reactive groups, idealized step-growth polymeric gels can be readily formed through bioorthogonal strain-promoted azide-alkyne cycloaddition (SPAAC) (Fig. ) . Taking advantage of crosslinkers designed to rapidly photolyze in a cytocompatible and visible wavelength-selective manner, we anticipated being able to achieve multiplexed material degradation in the presence of living cells and through complex tissue. Novel crosslinkers Rubiq (pink heptagon), Rubpy (green hexagon), and oNB (blue pentagon) undergo photolysis. Upon absorption of a photon, each ruthenium complex undergoes ligand exchange via population of a triplet metal-centered state via intersystem crossing from the low lying metal-to-ligand charge transfer (MLCT) band. This results in radical-free metal-ligand bond cleavage. Crosslinkers are modified with two azides for direct incorporation into hydrogel networks. b. Absorbance spectra of Rubiq, Rubpy, and oNB. Each crosslinker exhibits an extended absorbance spectrum beyond their lmax permitting excitation at wavelengths lower than lmax. c. PEG-based hydrogel formation occurs spontaneously upon mixing each crosslinker with 4-arm PEG-BCN via strain-promoted azide-alkyne cycloaddition. Resulting hydrogels degrade under red, green, or blue light with perfect unidirectional orthogonality (>617 nm for Rubiq, >530 nm for Rubpy, and >405 nm for oNB).