Eight novel 3-(4-(benzyloxy)phenyl)-5-(4-bromophenyl)-1-(4-substituted-phenyl)formazan (4a 4h) were synthesized by coupling of substituted phenylhydrazones with diazonium salts of 4-bromoaniline. The substituted phenylhydrazones, which are intermediate products, were obtained from the condensation of substituted phenylhydrazines with 4-(benzyloxy)benzaldehyde. All target compounds were characterized by using FTIR, H-1 NMR, C-13 NMR, LC-MS spectrometry, and elemental analysis. Absorption spectra of these compounds in solvents with different polarities were investigated thoroughly. Time-dependent density functional theory (TD-DFT) studies were conducted to shed light on their electronic structures, Kohn-Sham orbitals, and electronic transitions.