Abstract: In this work, zirconyl molybopyrophosphate with good cesium adsorption performance was synthesized under different experimental conditions. The adsorption properties of zirconyl molybopyrophosphate and zirconyl pyrophosphate were compared. The adsorption mechanism of cesium by zirconyl pyrophosphate was studied. With enough zirconyl and when the ratio of pyrophosphate to molybdate was 8∶1, zirconyl molybopyrophosphate with the best adsorption property was synthesized. Compared with zirconyl molybopyrophosphate, the adsorption performance of zirconyl pyrophosphate, which has a higher static adsorption capacity, is less affected by the solution acidity. Zirconyl pyrophosphate and zirconyl molybopyrophosphate have similar chemical stabilities. The adsorption mechanism involves ion exchanges between hydrogen ions of hydroxyl radical and cesium ions and is chemical adsorption.