A new zinc complex bis(benzyltriethylammonium) bis(1,3-dithiole-2-thione-4,5-dithiolato)-zinc(II) has been synthesized, its crystal structure has been determined by means of X-ray single crystal diffraction. The central zinc(II) ion coordinates with two ligands which constructed a distorted tetrahedron environment, cation groups and ligands link each other through weak intermolecular C-H center dot center dot center dot S hydrogen bonds. Its two-photon absorption properties has been studied using open aperture Z-scan technique with 14 ps pulses at wavelength 532 nm, its two-photon absorption cross section sigma(2) value was determined to be 8.73 x 10(-53) (m(4).s/photon.molecule). The theoretical mechanism of the two-photon absorption process was analysized by simplied five-energy-band model. (C) 2014 Elsevier B.V. All rights reserved.