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Waste concrete powder was used to remove fluoride ions in highly concentrated fluoride wastewater. 92.6% of fluoride in 100 mg F/L wastewater was removed by 1% dose of the cement paste powder that represents characteristics of waste concrete powder, whereas the removal efficiencies of raw cement and lime were 47.3% and 96.4%, respectively. The cement paste powder was competitive to lime, common fluoride removal agent. Various Ca-bearing hydrates such as portlandite, calcium silicate hydrate, and ettringite in cement paste slurry can remove fluoride by precipitating CaF2 and absorbing F- ions. In the experiments using both cement paste and lime, 50∼67% of lime can be substituted by cement paste to satisfy fluoride effluent limitation of 15 mg/L. Since cement paste has higher acid neutralization capacity than lime, it can be recycled to neutralize more acid and to remove more fluoride. Therefore waste concrete powder can be more economical and viable alternative for lime in fluoride wastewater treatment.