(A) Schematic shows how azobenzene residues are incorporated in the DNA sticky end, such that the trans (left) and cis (right) states of the azobenzene molecules can be toggled via visible or UV light, respectively. Under visible light (trans-form), the DNA sticky ends remain hybridized, but under UV light, the cis-form azobenzene molecules induce dehybridization of the DNA sticky ends. (B) Under isothermal conditions, light is applied to trigger a reversible change in PAE crystals between assembled and disassembled states. (C) UV-light-directed disassembly of surface-grown, crystalline PAE thin films can be used to selectively remove nanoparticles.