A reclaimable adsorbent of fungus hyphae-supported alumina (FHSA) bio-nanocomposites was developed, characterized and applied in fluoride removal from water. This adsorbent can be fast assembled and disassemble reversibly, promising efficient reclamation and high accessible surface area for fluoride adsorption. Adsorption experiments demonstrate that the FHSA performed well over a considerable wide pH range of 3–10 with high fluoride removal efficiencies (>66.3%). The adsorption capacity was 105.60mgg−1 for FHSA, much higher than that for the alumina nanoparticles (50.55mgg−1) and pure fungus hyphae (22.47mgg−1). The adsorption capacity calculated by the pure content of alumina in the FHSA is 340.27mgg−1 of alumina. Kinetics data reveal that the fluoride adsorption process on the FHSA was fast, nearly 90% fluoride adsorption can be achieved within 40min. The fluoride adsorption on the FHSA is mainly due to the surface complexes formation of fluoride with AlOH and the attraction between protonated NH2 and fluoride through hydrogen bonding. Findings demonstrate that the FHSA has potential applicability in fluoride removal due to its strong fluoride adsorbility and the easy reclamation by its fast reversible assembly and disassembly feature.