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Six Zn-Ln coordination complexes, [Nd 2 Zn 2 (C 6 H 5 COO) 10 (Imh) 2 (H 2 O) 2 ] ( 1 ), [Pr 2 Zn 2 (C 6 H 5 COO) 10 (Imh) 2 (H 2 O) 2 ] ( 2 ), [ErZn 2 (C 6 H 5 COO) 7 (Imh) 2 ] ( 3) , [HoZn 2 (C 6 H 5 COO) 7 (Imh) 2 ] ( 4 ), [EuZn 2 (C 6 H 5 COO) 7 (Imh) 2 ] ( 5 ), [TbZn 2 (C 6 H 5 COO) 7 (Imh) 2 ] ( 6 ) (C 6 H 5 COOH=benzoic acid, Imh=imidazole) have been synthesized under hydrothermal conditions and their crystal structures have been characterized by single crystal X-ray diffraction. All complexes are crystallized in triclinic system, with space group P ī. Complexes 1 and 2 are isomorphous with tetranuclear molecular structure and complexes 3–6 are isomorphous and trinuclear molecular complexes. All complexes are characterized by IR, UV–Vis–NIR and luminescent spectra in the visible and near-infrared (NIR) regions at room temperature. The study of luminescent properties indicates that all complexes exhibit the characteristic emission bands of corresponding Ln(III) ions, which should be attributed to sensitization from d-block and ligands after introducing Zn(II) ion and ligands into the system of Ln(III) complexes. Moreover, the NIR emission bands of complexes 1–4 exhibit shift and split, which can be evidenced in their UV–Vis–NIR absorption spectra. [ABSTRACT FROM AUTHOR]