Seven ferrocenyl schiff base organometallic compounds with third-order nonlinear optical properties which had large π-conjugated systems were designed and synthesized starting from ferrocene and substitutional amine. The process of reactions were discussed and the conditions of the reactions were selected. The results showed that the optimal parameters were as follows: catalyst alkaline Al2O3, solvent xylene, reflux 10 h. The yield was 59.1% .The influence of different substituted amine on the reaction yield was compared. It was concluded that the amine with more intense basicity give the higher yield. All the compounds were characterized by 1H NMR，MS and UV．The synthetic methods were simple and feasible.