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Three complexes of bifunctional 5‐substituted tetrazolatecarboxylate ligands [2‐(5‐(pyrazin‐2‐yl)‐2H‐tetrazol‐2‐yl)acetic acid (Hpztza), 3‐(5‐amino‐2H‐tetrazol‐1(5H)‐yl)propanoic acid (Hatzp), and N,N′‐bis(tetrazol‐5‐yl)anime‐N2,N2′‐diacetic acid (H2datza)], namely a mononuclear structure [La(pztza)2(H2O)5]·4H2O·pztza (1), a 1D polymeric chain structure [La2(atzp)4(H2O)8]·2NO3·2H2O (2), and a 2D layer network [La(datza)(H2O)3]·4H2O (3) were prepared and structurally characterized by elemental analysis, IR spectroscopy, and single‐crystal X‐ray diffraction. The structures of these complexes are controlled not only by the number and different coordination modes of the tetrazole‐carboxylate ligands but also the different 5‐substituents of the tetrazole ring. The complexes show ligand‐centered luminescence at room temperature in the solid state. The obvious enhancements in luminescence make these complexes to be the potential materials for optical use.

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Reactions of four different tetrazole‐containing carboxylic acids with GdCl3·6H2O, produced the coordination compounds, [Gd4(pytza)5(H2O)10(μ‐O) Cl]·4H2O·2Cl (1) [pytza = 2‐(5‐(pyridine‐4‐yl)‐2H‐tetrazole‐2‐yl)acetato], [Gd(pztza)2(H2O)6]·pztza·3H2O (2), [pztza = 2‐(5‐(pyrazin‐2‐yl)‐2H‐tetrazol‐2‐yl) acetato], [Gd(pmtza)2(H2O)6]Cl·2H2O (3), [pmtza = 2‐(5‐(pyrimidyl‐2‐yl)‐2H‐tetrazol‐2‐yl) acetato], and Gd(tzpya)2(H2O)5]Cl·4H2O (4) [tzpya = 2‐(4‐(5H‐tetrazol‐5‐yl)pyridin‐1(4H)‐yl) acetato]. The compounds were structurally characterized by elemental analysis, IR spectroscopy, and single‐crystal X‐ray diffraction. X‐ray diffraction analysis reveals that compound 1 displays a 2D single layered network and compounds 2–4 are mononuclear. Compounds 1–4 are self‐assembled to form 3D networks by hydrogen bonding interactions. Furthermore, the luminescent properties in the solid state at room temperature were investigated.