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Three novel metal-organic complexes with formulas [Ni(C9N2O2H7)2(CH3OH)2](1), [Zn(C9N2O2H7)2(H2O)2] (2) and [Cd(C9N2O2H7)2(CH3OH)2] (3) were synthesized by the reactions of Ni, Zn and Cd salts with ethyl 2-benzimidazolylacetate under hydrothermal conditions or layering technique, and characterized by single-crystal X-ray diffraction analysis, IR spectroscopy, solid-state luminescent properties and thermogravimetric (TG) analysis. The crystal data for these three complexes are as follows: for 1, monoclinic, space group P21/c, a = 9.384(3), b =9.634(3), c = 11.292(3) (A),β= 95.787(5)°, V= 1015.7(5)(A)3, Z= 2, F(000) = 492, Dc= 1.547 Kg/m3,μ = 1.002 mm-1, the final R = 0.0451 and wR = 0.0900 for 1833 observed reflections with I＞ 2σ(I);for 2, orthorhombic, space group Pbca, a = 10.031(4), b = 10.379(4), c = 17.525(7) (A), V =1824.6(12)(A)3, Z = 4, F(000) = 928, Dc= 1.645 Kg/m3,μ = 1.392 mm-1, the final R = 0.0452 and wR = 0.0996 for 1661 observed reflections with I ＞ 2σ(I); for 3, monoclinic, space group P21/c, a =9.9114(13), b =10.4852(15), c = 10.4120(14) (A),β= 108.453(5)°, V= 1026.4(2) (A)3, Z = 2, F(000) =532, Dc= 1.705 Kg/m3,μ = 1.110 mm-1, the final R = 0.0322 and wR = 0.0805 for 1822 observed reflections with I ＞ 2σ(I). In the three complexes, the ethyl 2-benzimidazolylacetate shows the same chelating mode, and the adjacent units are interlinked into a two-dimensional layer through hydrogen-bonds(O-H…O,N-H…O).