In this study, we investigated the removal of phosphate from aqueous solutions using (vinylbenzyl)-trimethylammonium chloride (VBTAC) grafted onto poly(ethylene terephthalate) (PET) fibers (PET-g-VBTAC). Batch-mode experiments were conducted using various contact times, initial phosphate concentrations, temperatures, pH values, and competing anions, to understand phosphate sorption onto PET-g-VBTAC. The phosphate sorption capacity of PET-g-VBTAC increased with increasing solution pH and was highest near pH 7. The equilibrium data fitted the Langmuir isotherm model well. The maximum sorption capacity (qm) of PET-g-VBTAC for phosphate was 55.6-56.0 mg/g at 25-45 °C. The sorption process followed a pseudo-second-order kinetic model. The obtained values of the mean free energy indicated that sorption of phosphate on PET-g-VBTAC occurs via ion exchange. Thermodynamic parameters, enthalpy change, entropy change, and Gibb's free energy, confirmed that phosphate sorption was spontaneous and endothermic. The adverse effects of competing anions on phosphate removal by PET-g-VBTAC were insignificant. These results demonstrate that PET-g-VBTAC effectively removes phosphate from aqueous solutions by ion exchange.