One of the parameters that impact on fluoride sorption capacities of materials in water defluoridation is initial concentration. Water from various sources will have different fluoride concentrations; as such the employment of a particular media in defluoridation requires information on how the media will perform in different concentrations. Consequently, research was carried out to determine how initial fluoride concentrations in raw water affect capacity in defluoridation with bauxite, gypsum, magnesite and their composite, and to investigate the possibility of predicting loading capacity of their composite filter through initial fluoride concentration to optimize their application in defluoridation. The results showed that sorption capacities increased with increase in initial concentrations. However, higher starting concentrations resulted in larger residual fluoride concentrations; as such the benefit of large sorption capacities obtained was overshadowed. Polynomial relations of capacity (Cs, mg/g) and initial concentration (Co, mg/l), were obtained for bauxite and gypsum. Magnesite obtained a logarithmic relation for Cs and Co. A power relation was obtained between Cs and Co for their composite, Cs = 0.0328C1.20160. Approximation of capacities of this composite from initial fluoride concentrations was feasible. Water defluoridation has become important as a result of dental and skeletal fluorosis.