 This paper presents the synthesis and characterization of four new Mn2, Fe3, and Cr3 complexes with two shift-based ligands, four Bromo2-E-4-2-hydroxyethylphenol-imeno-methylphenol-HL1 and 2-E-4-2-hydroxyethylphenol-imeno-methyl-4-methxyphenol-HL2. The ligands and their complexes were characterized by various analytical and spectroscopic methods including elemental analysis IR, 1-HNMR, 13-CNMR, mass spectra, magnetic susceptibility measurements, and X-ray crystallography. The general formulae of ML, CL2, H2O, 2-4-FEL1, CRL1 and CRL2 and ML, CL, H2O, 3-4-MnL2 were proposed. The optimized lowest energy configurations of the complexes were proven through DFD-B3-LYP calculations with Gaussian 0.9 program. This article was authored by Leila H. Abdulrahman, Emanieh Abdelgani, Abia Olabade, and others.