In this study, we prepared novel adsorbents containing virgin and calcined tapioca products for removing strontium (Sr(II)) and cesium (Cs(I)) from aqueous solutions. The characteristics of tapioca, along with its capacity to adsorb Sr(II) and Cs(I), were evaluated. Multiple tapioca products were prepared and tested. The adsorbent prepared by boiling the tapioca followed by calcination at 300°C (BTP300) was the most effective. In addition, adsorption was affected by the adsorbent’s surface properties. The Sr(II) and Cs(I) adsorbed onto BTP300 could be recovered through desorption by hydrochloric acid at different concentrations, which indicates that BTP300 can be used several times for adsorption/desorption. The results of this study suggest that BTP300, which was produced from tapioca biomass, can remove Sr(II) and Cs(I) from aqueous solutions.