Binderless mordenite zeolite with small crystal size of 100~200nm in c-axis direction was successfully prepared by a hydrothermal transformation method. The pre-formed precursor of aluminosilicate embedded with mordenite zeolite crystal seeds was converted into binderless mordenite zeolite with regular macro-morphology, high crystallinity and excellent mechanical stability. The catalyst for amination of ethanolamine to prepare ethylenediamine was developed based on the as-prepared binderless mordenite zeolite. The as-prepared catalyst exhibited good catalytic activity and selectivity for ethylenediamine due to high surface acidity and abundant porosity. At the reaction temperature 330~340 ℃, ethanolamine LHSV 0.40 h-1, n (NH3): n (MEA) =30, reaction pressure 1.8MPa, the catalyst stability test indicated that single pass conversion of MEA is about 50% and EDA selectivity is more than 70%, the total yield of EDA and PIP is about 40%. The catalyst remained stable for 1400 hours at the optimum reaction conditions. The activity of the catalyst recovered well after regeneration.