The present study reports a novel approach for synthesis of Zr nanoparticles using aqueous extract of Aloe vera. Resulting nanoparticles were embedded into chitosan biopolymer and termed as CNZr composite. The composite was subjected to detailed adsorption studies for removal of fluoride from aqueous solution. The synthesized Zr nanoparticles showed UV-vis absorption peak at 420 nm. TEM result showed the formation of polydispersed, nanoparticles ranging from 18 nm to 42 nm. SAED and XRD analysis suggested an fcc (face centered cubic) Zr crystallites. EDAX analysis suggested that Zr was an integral component of synthesized nanoparticles. FT-IR study indicated that functional group like -NH, -C=O, -C=N and -C=C were involved in particle formation. The adsorption of fluoride on to CNZr composite worked well at pH 7.0, where similar to 99% of fluoride was found to be adsorbed on adsorbent. Langmuir isotherm model best fitted the equilibrium data since it presented higher R-2 value than Freundlich model. In comparison to pseudo-first order kinetic model, the pseudo-second order model could explain adsorption kinetic behavior of F- onto CNZr composite satisfactorily with a good correlation coefficient. The present study revealed that CNZr composite may work as an effective tool for removal of fluoride from contaminated water. (C) 2014 Elsevier B.V. All rights reserved.