The organic-inorganic hybrid salt: 1, 1 -methylenedipyridinium pentacynidonitrosoferrate(II)pentahydrate is synthesized and characterized by multinuclear NMR, IR, and UV-vis spectroscopies and elemental analysis. The third order nonlinear optical properties of the new complex in an aqueous solution have been studied using Z-scan technique. Measurements were performed for input intensities (I0) of 437 and 241 W/cm 2 for the two concentrations with a CW diode laser at 635 nm wavelength. The nonlinear optical absorption coefficient (β) and nonlinear refraction (n2) are found at 1.28 × 10 −3 cm/W and 10.17 × 10 −9 cm 2 /W, respectively. The overall results suggested that better nonlinearity was observed at a higher concentration of sample. Our results suggest that this material is considered as a promising candidate for future optical device applications.