The invention discloses a monoethanolamine intramolecular dehydration catalyst. The carrier of the catalyst is acid activation montmorillonite. The active component of the catalyst is CsXY<c>O<d>, wherein X is phosphorus element, iron element or boron element, Y is rare earth element, O is oxygen element, a, b, c and d are the molar ratios of Cs, X, Y and O, and when a=1, b=0.5-2, c=0.2-1, and d is determined based on a, b and c. The acidity of the catalyst is regulated by means of the acid activation montmorillonite and phosphides, iron compounds or borides, the alkalinity of the catalyst is regulated by means of the rare earth element and Cs, the obtained catalyst is used for monoethanolamine intramolecular dehydration reaction to synthetize aziridine, and the conversion rate of monoethanolamine and the selectivity of aziridine can be improved at the same time.