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Hydrogen-bond-directed supramolecular assemblies of designed phosphonic acids are interesting examples of molecular tectonics.Here we report the crystallization of hexamethylenediamine-N,N,N',N'-tetrakis(methylenephosphonic acid)(labeled as H8L)in the absence or the presence of a templating agent(tetrabutylammonium),which afforded two new crystals,namely H8L(1)and [(NBu4)(H7L)](2),respectively.