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The detection of excess toxic anions or cations in an aqueous solution through various fluorescent materials such as organic or inorganic fluorescent materials has aroused significant interest recently. Herein, a new tetraimidazole ligand 1,3-bis(1-imidazolyl)-5-[3,5-bis(1-imidazolyl)-phenoxymethyl]-benzene (timpb) and its two Cd(II) metal–organic frameworks {[Cd2(1,4-bdc)2(timpb)]·5.5(H2O)}n (1) (1,4-benzenedicarboxylic acid = 1,4-H2bdc) and {[Cd2(4,4′-bpdb)2(timpb)]·(MeCN)·2.5(H2O)}n (2) (4,4′-biphenyldicarboxylic acid = 4,4′-H2bpdb) were synthesized. Through X-ray single crystal diffraction analysis, 1 can be considered as a 2-fold interpenetrating pillared-bilayer framework formed by linking [Cd2(1,4-bdc)4]n layers with pairs of timpb ligands, whereas 2 exhibits a 2-fold interpenetrating 3D honeycombed framework formed by linking [Cd(4,4′-bpdb)]n chains with timpb ligands. The solid-state luminescent properties of timpb, 1 and 2 at ambient temperature were also investigated. Moreover, timpb acted as a potential luminescent sensor for the detection of cations Fe3+ or Cu2+ and the anion Cr2O72−, whereas 1 displayed high sensitivity toward the cation Fe3+ and anion Cr2O72−. [ABSTRACT FROM AUTHOR]