Five of ferrocenyl organometallic compounds have been synthesized with phase-transfer Wittig reaction and characterized by IR, UV, elemental analysis and 1 HNMR. The crystal X-ray structure and nonlinear second-order optical properties of the compounds have been studied. It is concluded that this kind of compounds have fairly large second-order susceptibility, and that, both donor-acceptor substi-tutes and the extending conjugated area facilitate the nonlinear second-order optical susceptibility.