Phosphorus contamination in fresh water has posed a great risk to aquatic ecosystems and human health due to extensive eutrophication. In this paper, we are reporting a lanthanum (La)-modified aminated polyacrylonitrile (PAN) adsorptive membrane for effective decontamination of phosphorus from the simulated water. The PAN membrane was first aminated to introduce the amine group as an active site for La and then followed by the in situ precipitation of La particles. The kinetics study showed that the rapid adsorption occurred within the initial 4 h with the equilibrium established at 8 h. The membrane worked well in the acidic pH region, with optimal pH 4 and 5 without and with the pH control, respectively. The maximum adsorption capacities were 50 and 44.64 mg/g at pH 5 and 7, respectively. The adsorption of phosphorus was not affected by the existence of commonly existing anions except fluorides in water. In the filtration study, it was observed that the removal of phosphorus remained the optimum, although the operating pressure was increased from 1 to 3 bar. The modified membrane was able to treat 0.32 L of a 10 mg/L phosphate solution to meet the maximum allowable limit of 0.15 mg/L for the trade effluent. The mechanism study revealed that the removal was primarily associated with the ion exchange between a phosphorus ion and a hydroxyl group from the La particles.