This paper presents findings of a study on optimization and application of the regenerated bone char media for the defluoridation of drinking water in Tanzania where more than 30% of all water sources have fluoride concentrations above the 1.50 mg/l which is recommended by the World Heath Organization (WHO). In this study, regeneration temperature, regeneration duration, contact time, regenerated bone char dosage and particle size were investigated. Results indicate that the highest fluoride removal and adsorption capacity were 70.64% and 0.75 mg-F/g-bc, respectively, for a sample with bone char material that was regenerated at 500°C. In this study the optimum burning duration was found to be 120 min, which resulted in residual fluoride that varied from a maximum value of 17.43 mg/l for a 2 min contact time to a minimum value of 8.53 mg/l for a contact time of 180 min. This study further indicated that the smallest size of regenerated bone char media (0.5–1.0 mm diameter) had the highest defluoridation capacity, with residual fluoride which varied from 17.82 mg/l at 2 min contact time to 11.26 mg/l at 120 min contact time. In terms of dosage of the regenerated bone char media it was established that the optimum dosage was 25 g of bone char media with a grain size of 0.50–1.0 mm. This had a fluoride removal capacity of 0.55 mg-F/g-BC. Column filter experiments indicated that regenerated bone media is capable of removing fluoride from dinking water to meet both WHO and Tanzania recommended values.