Recently, the high‐concentration phosphorus‐containing wastewater has been caused lots of negative influences on aquatic environment and thus driven people to develop some effective methods to remove excess of phosphate in water. In order to solve these environmental problem, in this work, a tetraethylenepentamine (TEPA) modified 4A zeolite has been prepared and used for removing phosphate. Removal of phosphate by precipitation of 4A zeolite and electrostatic action of TEPA with phosphate were determined by scanning electron microscopy, X‐ray powder diffraction and Fourier infrared spectrum, and morphology and characteristic peak of TEPA‐4A zeolite before and after adsorption changed significantly. In addition, the results of batch adsorption studies showed that the pH of the solution have a significant influence on the adsorption of TEPA‐4A and the biggest adsorption capacity was 23 mg/g at pH = 2.3 ± 0.2. Adsorption isotherms results showed that the process was consistent with Langmuir model and the maximum adsorption capacity could reach to 28 mg/g at 25 °C. TEPA‐4A adsorption processes were spontaneous endothermic reaction, and elevated temperatures were conducive to the adsorption process through kinetics and thermodynamics results. The research of TEPA modified 4A zeolite and raw 4A zeolite provides technical support for the development of 4A zeolite instead of sodium tripolyphosphate as a new type of detergent ingredient.