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The self-assembly of π-aromatic organic and organometallic molecules into long-range-ordered supramolecular polymers is dictated by a variety of molecular parameters and external conditions. In this work, structural isomerism, representing one of the potent molecular parameters, has been investigated to modulate the self-assembly behaviors. Two platinum(II) acetylide-based structural isomers, with different N-hexyl substitution positions on the inner benzotriazole core, have been designed. Thanks to the synergistic participation of hyd