The invention provides a method for synthesizing pollucite by means of an aluminosilicate polymer.The method comprises the steps that cesium hydroxide and sodium hydroxide are dissolved in silica sol with the mass concentration of 25%-45%, mechanical stirring is conducted, and a mixed alkali-activated solution of cesium silicate and sodium silicate is obtained; kaolin is put into an alumina crucible, the alumina crucible containing kaolin is put into a muffle furnace, the temperature is set to range from 500 DEG C to 900 DEG C, the heat preservation time ranges from 1.5 h to 2.5 h, and metakaolin powder is obtained; the mixed alkali-activated solution is put into an ice-water bath with the temperature ranging from 0 DEG C to 5 DEG C, the metakaolin powder is added, ultrasound treatment and mechanical stirring are conducted for 25 min-45 min, an aluminosilicate polymer slurry is obtained, deionized water is added to adjust the viscosity of the slurry to be 150 mPa.s-500 mPa.s when the shearing speed is 60 S<-1>-80 S<-1>, and the aluminosilicate polymer slurry is obtained; the obtained aluminosilicate polymer slurry is poured into a mold and cured for 3 h-24 h in a drying oven with the temperature ranging from 40 DEG C to 80 DEG C, and then pollucite is obtained.