A novel ligand (H2L), diethylenetriamine-N,N′,N′′-triacetylisoniazide N,N′′-bisacetic acid, and its four non-ion transition metal complexes, ML · nH2O (M = Mn, n = 4; M = Co, Ni, n = 2; M = Cu, n = 1), have been synthesized and characterized on the basis of elemental analysis, molar conductivity, 1H-NMR, FAB-MS, TG-DTA analysis and IR spectrum. In addition, relaxivity (R1) of the complexes was determined, the relaxivity of MnL, CoL, NiL, CuL as well as Gd(DTPA)2− used as a control are 6.94, 2.79, 2.52, 1.59 and 4.34 l mmol−1 s−1, respectively. The relaxivity of MnL is larger than that of Gd(DTPA)2−. The results show that the complex of MnL may be a potential MRI contrast agent.