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We realized the fabrication of a new kind of supramolecular organometallic gels with a discrete rhomboidal metallocycle as the main skeleton via hierarchical self-assembly.More importantly, by taking advantage of the dynamic nature of metal-ligand bonds, the stimuli-responsive gel-sol transition of the obtained gels was realized via disassembly and reassembly of the rhomboidal scaffold as controlled by bromide ions.