The new functional material, the hybrids with molecular formula (C6H5CNH2nNH3)2PbI4(where N=0,1,2) were synthesized by reactions in solution. The influences of the reactant ratio and the reaction time on the structures of the products were investigated. The structures and the properties of the hybrids were characterized using X-ray diffraction(XRD), scanning electron microscopy (SEM) and ultraviolet&visible (UV) adsorption spectra . The effect of number of methylene, n, on the structure forming and the band gap magnitude has been studied. The results demenstrate that the number of methylene has effect both on the forming of the layered structure and on the magnitude of the band gap.