This study evaluates the application of denim fiber scraps as a precursor for the synthesis of adsorbents for water treatment via pyrolysis and their application in water defluoridation. The best pyrolysis conditions for the synthesis of this novel adsorbent have been identified and a metal doping route with different salts of Al 3+ , La 3+ and Fe 3+ was proposed to improve its fluoride adsorption behavior. Different spectroscopic and microscopic techniques (i.e., FTIR, XPS, XRF, SEM) were used to characterize the precursor and adsorbents, and to analyze the surface interactions involved in the fluoride removal mechanism. Experimental results showed that these adsorbents were effective for fluoride adsorption showing uptakes up to 4.25 mg/g. The Si-Ometal-F interactions appear to be highly relevant for the fluoride removal. This study highlights the potential of denim textile waste as a raw material for the production of added-value products, thus minimizing their associated disposal cost. It also highlights the performance of denim textile waste as a precursor of adsorbents for addressing relevant environmental concerns such as fluoride pollution.