The spherical Resorcinol-Formaldehyde and hypothetical spherical SuperLig (R) 644 ion-exchange resins are evaluated for cesium removal from radioactive waste solutions. Modeling results show that spherical SuperLig (R) 644 reduces column cycling by 50% for high-potassium solutions. Spherical Resorcinol Formaldehyde performs equally well for the lowest-potassium wastes. Less cycling reduces nitric acid usage during resin elution and sodium addition during resin regeneration, thereby significantly decreasing life-cycle operational costs. A model assessment of the mechanism behind cesium bleed is also conducted. When a resin bed is eluted, a relatively small amount of cesium remains within resin particles. Cesium can bleed into an otherwise decontaminated product in the next loading cycle. The bleed mechanism is shown to be fully isotherm-controlled vs. mass transfer controlled. Knowledge of residual post-elution cesium level and resin isotherm can be utilized to predict rate of cesium bleed in a mostly non-loaded column. Overall, this work demonstrates the versatility of the ion-exchange modeling to study the effects of resin characteristics on processing cycles, rates, and cold chemical consumption. This evaluation justifies further development of a spherical form of the SuperLig (R) 644 resin.