Since the aggregates resulted from the co-assembly of AzoDiGua with ATP, we explored the challenge to realize the first photoreversible ATP-based supramolecular assemblies. Indeed, pure AzoDiGua is able to reversibly photoisomerize between trans and cis upon UV and blue light irradiation, respectively (Figure ) . To characterize the photoresponse of the supramolecular aggregates, we first prepared the ATP/AzoDiGua aggregates in the regular conditions ([ATP] = 1 mM, [AzoDiGua] = 1 mM, 10 min incubation at room temperature) using pure trans-AzoDiGua as a starting material and exposed them to successive irradiations by UV (395/25 nm, 26 mW•cm -2 ) for 3 min and blue (480/30 nm, 40 mW•cm -2 ) for 3 min. The first UV application resulted in the progressive disassembly of the supramolecular aggregates until their complete disappearance in less than 1 min (Movie S2, Figure ). The subsequent blue irradiation led to the recovery of the assembly with a similar kinetics (Movie S2, Figure ). This was accompanied by a photocontrol of the optical properties of the ATP/AzoDiGua suspension. The first UV irradiation led to the loss of the suspension turbidity due to the vanishing of the light-scattering entities and appearance of the characteristic color of the cis-AzoDiGua isomer enriching the solution (Figure middle, Figure ). Similarly, the subsequent exposure to blue irradiation induced a change of the optical aspect of the suspension which became turbid again, due to the reappearance of the micrometer-sized ATP/AzoDiGua aggregates (Figure right). Note that, compared to the initial suspension composed of pure trans-AzoDiGua, the suspension after UV and blue irradiation was less turbid and the aggregates in smaller number and with a smaller size due to an incomplete trans-isomer enrichment upon blue irradiation in the photostationary state . This successive disassembly/reassembly of the ATP/AzoDiGua aggregates upon UV/blue irradiation was then successfully repeated for five complete consecutive cycles (Figure ). It resulted in a dynamic and reversible photocontrol of the suspension fluorescence correlating with the assembly state, i.e., high intensity for the blue-induced assembly and low intensity after UV-induced disassembly, respectively, with only small fatigue appearing from the third cycle (Figure ).