Lanthanum impregnated chitosan/beta-cyclodextrin (CS-La-beta CD) composite was prepared using a facile in situ fabrication method and successfully evaluated for the adsorption of CrO42- and F-. The pristine and treated CS-La-beta CD was characterized using Fourier transform infrared, scanning electron microscopy, energy dispersive X-ray spectroscopy with mapping, X-ray diffraction, and thermal gravametric analytical techniques. The optimum conditions for the uptake of CrO42- and F- were investigated as a function of shaking time, dosage, initial ion concentration, pH, and predatory ions in batch experiments. The equilibrium data were fitted using Langmuir, Freundlich, and Dubinin-Radushkevich models for the defluoridation and sorption of chromium onto CS-La-beta CD. The adsorption kinetics of CrO42- and F- followed the pseudo-second order model. The maximum Langmuir adsorption capacity was found to be 91.58 mg/g and 8.14 mg/g for CrO42- and F-, respectively at 303 K. Sequential adsorption and desorption studies were carried out up to five cycles using 0.1 M of NaOH as an eluent to check the reusability of the adsorbents.