Reconfigurable micro-nanostructures have been largely used in the development of modern photocontrol technology. In this work, a dynamically adjustable hydrogel of supramolecule structures is realized by molecule self-assembly and cross-link in microscale. Calculations based on the molecule modeling systematically illuminate the assembly process and the mechanism of the dynamically adjustable micro-nanostructure. The transmittance changes of the hydrogel, which are measured in the visible-light range before and after electric heating, show outstanding light-control function. Thus, the one-step fabrication, bio-compatibility (no initiator, cross linker, or monomer residual), and agile photocontrol application demonstrate the potential of the adjustable physically bonded hydrogel in development of low-loss and integrated dynamical light-control devices.