Ferrocenyl Schiff base derivatives [FcCHN(Ar)] (L1), [FcCOCH = C(NHAr)] (L2) (Fc = (C5H5)2Fe and Ar = [(2-OH)(p-C6H3NO2] and corresponding d10 metal complexes [L2M] [M = Zn (1), Cd (2)] have been synthesized and characterized by elemental analysis, FT-IR, 1H NMR, UV-Vis and emission spectroscopies. The electrochemical studies have examined that ligands and metal complexes show quasi-reversible redox wave which indicates electron transfer ability of ferrocene to nitro group via Schiff base (-C=N) conjugation group. Third-order nonlinear optical (NLO) properties were determined by Z-scan techniques in DMF solution. Complex 2 shows larger third order NLO susceptibility χ(3) (5.6×10-6 esu) than ligand L1 (1.6×10-6 esu) and L2 (3.1×10-6 esu). Hence, complex 2 is a promising candidate for NLO devices. © 2014 by American Scientific Publishers.