A new ecomaterial, zirconyl molybdopyrophosphate (ZMPP), was prepared by a coprecipitation method. The removal of Cs+ and Sr2+ ions from simulated strong acid HLLW using the ion exchange process on ZMPP had been investigated. It showed that there are more than 90% Cs+ and Sr2+ removed from the simulated HLLW on ZMPP despite the presence of other metal ions, such as Na+, Al3+, Fe3+, etc. in excess. Then ZMPP may likely be a selective ion exchanger for the removal of 137Cs and 90Sr directly from strong acid HLLW.