Molecular recognition is fundamental to the specific interactions between molecules, of which the best known examples are antibody antigen binding and cDNA hybridization. Reversible manipulation of the molecular recognition events is still a very challenging topic, and such studies are often performed at the molecular level. An important consideration is the collection of changes at the molecular level to provide macroscopic observables. This research makes use of photoresponsive molecular recognition for the fabrication of novel photoregulated dynamic materials. Specifically, a dynamic hydrogel was prepared by grafting azobenzene-tethered ssDNA and its cDNA to the hydrogel network. The macroscopic volume Of the hydrogel can be manipulated through the photoreversible DNA hybridization controlled by alternate irradiation of UV and visible light. The effects of synthetic parameters including the concentration of DNA, polymer monomer, and permanent cross-linker are also discussed.