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This technology is a programmable, CRISPR-based hydrogel with a wide range of abilities, including release of biomolecules or regulation of electric circuits, in response to specific DNA targets. The hydrogel is constructed using single-stranded DNA sequences as key structural elements or as linkers to cargo, such as fluorescent molecules. Following introduction of a user-defined, external DNA stimuli, a Cas enzyme and guide RNA (gRNA) complex cleaves the single-stranded DNA sequences in the hydrogel, leading to the restructuring of the polymeric material or release of the bound cargo. Importantly, this technology eliminates the need to encode target-sequence specificity into the gel structure. Instead, specificity of the Cas enzyme is easily modulated through simple replacement of the gRNA sequence. The inventors have demonstrated that a wide range of different payloads, including fluorescent molecules, active enzymes, and encapsulated nanoparticles and live cells, can be released from hydrogels at a controllable rate upon exposure to low concentrations of DNA stimuli. Furthermore, this smart biomaterial can act as a stimuli-responsive electric fuse and a controllable valve in fluidic devices.