ALT Recombinant protein-based biomaterials offer exciting opportunities in materials design and controlled therapeutic delivery. Though their precursors can be readily synthesized with near-perfect monodispersity and sequence specificity through scalable fermentation processes, recombinant protein materials have yet to achieve the same level of multi-stimuli-responsiveness as their synthetic counterparts. Integrating cutting-edge tools from chemical biology, we autonomously compile topologically specified protein crosslinkers that can be degraded following user-programmable Boolean logic. Covalent step polymerization of these linkers into protein hydrogels yields smart materials whose cargo (e.g., bioactive proteins, cellular therapeutics) can be liberated following bulk degradation in response to user-specified input combinations.