The synthesis of ashape-memory acrylamide-DNA hydrogel that includes two internal memories is introduced. The hydrogel is stabilized, at pH 7.0, by two different pHresponsive oligonucleotide crosslinking units.AtpH10.0, one of the T-A·T triplex DNAb ridging units is dissociated, resulting in the dissociation of the hydrogel into as hapeless quasi-liquid state that includes the other oligonucleotide bridges as internal memory.S imilarly,a tp H5.0, the second type of bridges is separated, through the formation of C-G·C + triplex units to yield the shapeless quasi-liquid state that includes the other oligonucleotide bridges as internal memory. By reversible pH triggering of the hydrogel between the values 10.0,7.0,5.0, the two internal memories cycle the material across shaped hydrogel and shapeless quasi-liquid states.T he two memories enable the pH-dictated formation of two different hydrogel structures.The design of stimuli-responsive DNA-based hydrogels attracts substantial recent interest. Thecrosslinking of nucleic acid-tethered polymer chains through the formation of duplex bridging units provides ag eneral means to generate DNAbased hydrogels.[1] Theh ydrogel-to-polymer solution transitions of these systems were induced by strand displacement, [2] temperature, [3] enzyme [3,4] or DNAzyme [5] cleavage of the bridging units.O ther DNA-based hydrogels undergoing cyclic and reversible hydrogel-to-polymer solution included metal-ion (e.g.,A g + )-induced bridging of duplex DNAa nd their separation by ligands eliminating the ions (e.g., cysteamine), [6] the pH-induced formation of i-motif-crosslinked hydrogels (at pH 5.2) and the separation of the i-motif structure at neutral pH, [7] the K + -ion-stimulated crosslinking of polymer chains by G-quadruplex units and the separation of the hydrogel by means of 18-crown-6-ether that eliminates the K + ions, [8] the use of light, [9] and the use of different Hoogsteen-type pH-sensitive triplex DNAa sb ridging units of the polymer chains.[10] Different applications of stimuliresponsive DNA-based hydrogels were suggested, including controlled drug release, [11] sensors, [12] switchable catalysis, [8] and catalyzed synthesis of conducting wires, [13] separation of substrates, [14] and the triggered activation of enzyme cascades. [5] Shape-memory polymers represent an interesting class of smart, stimuli-responsive materials.T hese polymers are processed into ap ermanent shaped structure that is programmed into at emporary shape that includes am emory to restore the original shape,i nt he presence of an appropriate trigger. [2,3,6,8,13a, 15] Avariety of triggers such as thermal, light or magnetic stimuli were used to activate shape-memory materials.[3,9,15f] Different applications of shape-memory materials were suggested, including their use as sensors, functional materials for inscription, [16] matrices for controlled drug release, [17] and materials for actuating microdevices.[18]Thei nformation encoded in oligonucleotide [19] sequences provides versatile means ...