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A novel soluble π-conjugated polymer, poly[(3-octanoylpyrrole-2,5-diyl)-p-(N,N-dimethylamino)benz ylidene] (POPDMABE), was synthesized firstly by the condensation of 3-octanoylpyrrole with paradimethylaminobenzaldehyde. The chemical structure of the polymer was characterized by FTIR and 1H NMR spectrometries. The polymer is a potential nonlinear optical(NLO) material. According to the function of optical forbidden band gap(Eg) and photon energy(hv), the optical forbidden band gaps of the polymer before and after ion implantation were calculated. The resonant third-order nonlinear optical properties of POPDMABE before and after ion implantation were also studied by using the degenerate four-wave mixing (DFWM) technique at 532 nm. When the energy is 25 keV and the dose is 2.2×1017 ions/cm2, the polymer's optical forbidden band gap is about 1.63 eV which is smaller than that of the non-implanted sample (1.98eV) and the resonant third-order NLO susceptibility of POPDMABE is about 4.3×10-7 esu, 1 order of magnitude higher than that of the non-implanted sample(4.1×10-8 esu). The results show that nitrogen ion implantation is an effective method to improve the resonant third-order NLO property of the polymer.