In this research, a new composite adsorbent consisting of zeolite Y and polyacrylonitrile (PAN) was synthesized. The composite was characterized by XRD, XRF, FTIR, DTG, and SEM analysis. The adsorption behavior of the composite toward Cs+ and Sr2+ was investigated. The effect of pH, initial ion concentration, contact time, and temperature on sorption process was examined. The maximum adsorption capacity of the composite was 219.8 and 70.23 mg g−1 for Cs+ and Sr2+, respectively. The kinetic of the process followed pseudo‐second‐order model. The equilibrium data were analyzed by the Langmuir, Freundlich, and D‐R isotherm models. The mean free energy of the sorption (E) for both ions was in the range of 8–16 kJ mol−1, confirming an ion exchange mechanism had been carried out. Positive ΔH° and negative ΔG° were indicative of the endothermic and spontaneous nature adsorption. Obtained results revealed the PAN‐NaY composite was a desirable ion exchanger for Cs+ and Sr2+ removal. © 2015 American Institute of Chemical Engineers Environ Prog, 34: 999–1008, 2015