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Abstract: A novel organic–inorganic hybrid complex [(2-NH2CH2C5H4N)ZnCl3] has been hydrothermally synthesized and characterized by single crystal X-ray diffraction, thermal analysis and spectroscopic studies. The compound crystallizes in the triclinic system, space group , a =7.5339(9), b =7.589(2), c =9.365(2) Å, α =104.55(2)°, β =97.22(1)°, γ =87.88(2)°, V =513.6(2), Z =2. In the title compound the 2-aminomethylpyridine acts as a ligand covalently linked to Zn(II) cation to form a slightly distorted ZnCl3N tetrahedral environment. Each [Zn(C6H8N2)Cl3] unit is connected to one neighbor by a pair of hydrogen bonds between the apical chlorides and amine hydrogen atoms and to the other by a couple of π–π stacking interactions between the aromatic rings of the coordinated ligands forming a novel one-dimensional chain-like arrangement. The title complex is the first one that contains both coordinated and hydrogen bonded 2-aminomethylpyridine. Solid state 13C and 15N CP-MAS-NMR spectroscopies are in agreement with the X-ray structure. Ab initio calculations allow the attribution of carbons and nitrogen to the independent crystallographic sites. The Raman spectroscopy confirmed the presence of Zn–Cl and Zn–N bonds. [Copyright &y& Elsevier]