Adenosine 5'-triphosphate (ATP) is involved in many biological and biotechnological processes, making its dynamic actuation, and especially by light, a valuable challenge for a broad range of applications of fundamental and/or practical interest. Instead of the conventional approach involving a covalent modification to render it stimulus-responsive, we have described an original strategy where ATP is associated with a photosensitive nucleotide binder called AzoDiGua to form multi-stimuli responsive supramolecular structures through non-covalent interactions. AzoDiGua is a water-soluble azobenzene molecule with two guaninidium groups as its extremity and known as a photosensitive DNA intercalator. Here, we exploited its phototunable capacity to interact with nucleotides through π-π and electrostatic interaction to build a new kind of photoresponsive co-assembly using ATP as a co-assembly partner. We showed in particular that simply mixing AzoDiGua and ATP led to the spontaneous assembly of the two partners into micrometer-sized aggregates in a few minutes in water. The interest of such an approach is multifold. First, the approach allows to dynamically control the assembly/release of ATP by light without having to modify it, and in mild conditions (physiological pH, room temperature, ATP concentrations similar to intracellular one), making the approach particularly robust, prone to generalization to other targets and opening interesting perspectives for in situ non-invasive actuation. Second, the non-covalent assembly allows to maintain the stimulus-responsiveness of the individual bricks in the supramolecular structure.