A method of purifying triethylene tetraamine hexamethylene phosphonic acid (TTHMP) is disclosed. The method includes dissolving a TTHMP crude product into water, adjusting the pH value by using an alkaline compound until reaching strong basicity, adding a poor solvent, allowing an oily compound to be separated from the bottom of the container, allowing the mixture to stand, collecting the oily compound, dissolving the collected oily compound with water, heating until refluxing, adding the poor solvent until a turbid phenomenon occurs, maintaining a refluxing state, adding water again until the solution is clear, stopping heating, allowing the solution to stand and be cooled, allowing an oily compound to be separated from the bottom of the container, collecting the oily compound, repeating the steps to collect the oily compound, dissolving the oily compound with water, adding an acidic compound to adjust the pH value to acidity, adding the poor solvent, allowing an oily compound to be separated from the bottom of the container, allowing the solution to stand, collecting the oily compound, washing the oily compound with a mixed solvent comprising water and the poor solvent, collecting the oily compound, and drying in a vacuum dryer to obtain white solid powder that is a purified TTHMP product. The method is used for separating impurities properties of which are similar in the TTHMP crude product. The yield of the final product is high, and purity is higher than 99%.