Zeolite was synthesized from power station waste, coal fly ash, as an alternative low-cost adsorbent and investigated for the removal of Sr(II) and Cs(I) ions from single- and binary metal aqueous solutions. In order to investigate the adsorption characteristics, the effects of various operating parameters such as initial concentration of metal ions, contact time, and pH of the solutions were studied in a batch adsorption technique. The Langmuir model better fitted the adsorption isotherm data than the Freundlich model. The pseudo second-order model was found more applicable to describe the kinetics of system. The adsorption capacities of Sr(II) and Cs(I) ions obtained from the Langmuir model were 1.7848 mmol/g and 0.7640 mmol/g, respectively. Although the adsorption capacities of individual Sr(II) and Cs(I) ions was less in the binary-system, the sum of the total adsorption capacity (2.3572 mmol/g) of both ions in the binary-system was higher than the adsorption capacity of individual ion in the single-system. Comparing the homogeneous film diffusion model with the homogeneous particle diffusion model, the adsorption was mainly controlled by the particle diffusion process.