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The reactions of substituted N-benzyliminodiacetamides (o-CH3Bnimda, m-CH3Bnimda, p-CH3Bnimda, o-ClBnimda, m-ClBnimda, p-ClBnimda, p-FBnimda, and p-BrBnimda; o-CH3Bn = ortho-methylbenzyl, m-CH3Bn = meta-methylbenzyl, p-CH3Bn = para-methylbenzyl, o-ClBn = ortho-chlorobenzyl, m-ClBn = meta-chlorobenzyl, p-ClBn = para-chlorobenzyl, p-FBn = para-fluorobenzyl, and p-BrBn = para-bromobenzyl) with copper(ii) and nickel(ii) nitrate in aqueous solutions were investigated. Sixteen new complexes [Cu(o-CH3Bnimda)2](NO3)20.5H2O (1), [Cu(m-CH3Bnimda)2](NO3)2 (2), [Cu(p-CH3Bnimda)2](NO3)2•2H2O (3), [Cu(o-ClBnimda)2](NO3)2H2O (4), [Cu(m-ClBnimda)2](NO3)2 (5), [Cu(p-ClBnimda)2](NO3)2•2H2O (6), [Cu(p-FBnimda)2](NO3)2•2H2O (7), [Cu(p-BrBnimda)2](NO3)2•2H2O (8), [Ni(o-CH3Bnimda)2](NO3)2H2O (9), [Ni(m-CH3Bnimda)2](NO3)2•2H2O (10), [Ni(p-CH3Bnimda)2](NO3)2H2O (11), [Ni(o-ClBnimda)2](NO3)2 (12), [Ni(m-ClBnimda)2](NO3)22DMF (13) (DMF = N,N-dimethylformamide), [Ni(p-ClBnimda)2](NO3)2•2H2O (14), [Ni(p-FBnimda)2](NO3)2H2O (15), and [Ni(p-BrBnimda)2](NO3)2•2H2O (16) were prepared and characterized by infrared spectroscopy and thermal analysis (thermogravimetric and differential thermal analyses). The molecular and crystal structures of three complexes (2, 5, and 13) were determined by X-ray crystal structure analysis. The octahedral coordination environments around the copper(ii) and nickel(ii) ions in complexes 2, 5, and 13 consist of two O,N,O'-tridentate iminodiacetamide ligands. The complexes are trans-isomers with fac-configuration of the chelators. [ABSTRACT FROM AUTHOR]