A method for synthesizing high-content NaY molecular sieves with kaolin sprayed microspheres includes adding functional components and deionized water into kaolin so as to be pulped into a mixed slurry. The slurry is sprayed into microspheres. The microspheres are calcined at a temperature between 700 and 1,000.degree. C. and mixed with a directing agent for crystallization. The resultant solid is filtrated and washed with water and then dried to obtain a final in-situ crystallized product with high content of molecular sieves.