A new Schiff base ligand derived from S-benzyldithiocarbazate and 4-[N-hydroxy ethyl-N-(methyl)amino]benzaldehyde (HL, where H is a dissociable proton) and its Ni-II, Cu-II, Zn-II and Pd-II complexes were prepared and fully characterized. The structures of HL and Ni(L)(2) were determined by X-ray diffraction analysis, which revealed that the geometry of the Ni-II ion is square-planar with two equivalent Ni-N and Ni-S bonds, and that the two neighboring molecules in two layers have weak contact. The electronic spectra and solution fluorescence of the ligand and the complexes were studied, and the quantum yields of single-photon fluorescence for the compounds were determined. The compounds possess two-photon absorption (t.p.a.) character and the t.p.a. coefficient beta and t.p.a. cross-section sigma were determined by the Z-scan technique. Especially, the Zn(L)(2) complex and the HL ligand exhibit intensive two-photon fluorescence (t.p.f.) at 800 nm laser pulses in the femtosecond regime.