In this work, a graphene oxide (GO)-filled polypropylene (PP) adsorptive membrane was developed through an environmentally benign plasma-treatment technology. The PP/GO composite membrane was prepared through melt-compounding and subsequent compression molding processing. The composite membrane was further modified through the plasma treatment with allylamine as the monomer. The results showed that the modified composite membrane exhibited a high hydrophilicity, which is attributed to the introduction of a large number of nitrogen-containing and oxygen-containing groups. The plasma assisted surface modification technology was applied to the porous composite membrane that was prepared through uniaxial stretching processing. Although the porosity of the porous membrane gradually decreased with increasing discharge time during the plasma treatment, the modified porous membrane exhibited an excellent adsorption ability. When adsorbing the particles from the solution, the amount of adsorbed Congo-red particles increased with increasing discharge time. The adsorption mechanism of the treated porous membrane was then analyzed. This work provides an efficient method to apparently improve the hydrophilicity and adsorption ability of a PP-based composite membrane which has great potential in the field of wastewater treatment.