Fluoride in drinking water above permissible levels is responsible for human dental and skeletal fluorosis. In this study, therefore, the large internal surface area of zeolite was utilized to create active sites for fluoride sorption by exchanging Na+-bound zeolite with Al3+ or La3+ ions. Fluoride removal from water using Al3+- and La3+-exchanged zeolite F-9 particles was subsequently investigated to evaluate the fluoride sorption characteristics of the sorbents. Equilibrium isotherms such as the two-site Langmuir (L), Freundlich (F), Langmuir–Freundlich (LF), Redlich–Peterson (RP), Tóth (T), and Dubinin–Radushkevitch (DR) were successfully used to model the experimental data. Modeling results showed that the isotherm parameters weakly depended on the solution temperature. From the DR isotherm parameters, it was considered that the uptake of fluoride by Al3+-exchanged zeolite proceeded by an ion-exchange mechanism (E=11.32−12.13 kJ/mol), while fluoride–La3+-exchanged zeolite interaction proceeded by physical adsorption (E=7.41−7.72 kJ/mol). Factors from the solution chemistry that affected fluoride removal from water were the solution pH and bicarbonate content. The latter factor buffered the system pH at higher values and thus diminished the affinity of the active sites for fluoride. Natural groundwater samples from two Kenyan tube wells were tested and results are discussed in relation to solution chemistry. In overall, Al3+-exchanged zeolite was found to be superior to La3+-exchanged zeolite in fluoride uptake within the tested concentration range.