Natural zeolite is organically modified with the surfactant cetyltrimethylammonium bromide (CTAB) and employed as a dual-function material for simultaneous adsorption of Cs+ cations and HCrO4− anions from aqueous solutions. Unmodified and modified zeolites are characterized by Fourier transform infrared (FTIR), dynamic light scattering (DLS), nitrogen adsorption–desorption isotherms, and X-ray diffraction (XRD). The results showed that CTAB-zeolite had the efficiency to simultaneously adsorb the concerned species in the pH range 2.5–4.2. The kinetic data showed that 90 and 300 min for Cs(I) and Cr(VI), respectively, were sufficient to attain equilibrium and the data are well-fitted by the double-exponential kinetic model. Of the studied adsorption isotherm models, Redlich-Peterson was the best one for describing the equilibrium adsorption isotherms. Values of ∆H°, ∆S°, and ∆G° for the present adsorption processes are estimated. CTAB-zeolite exhibited adsorption capacities of 0.713 and 1.216 mmol/g for Cs(I) and Cr(VI), respectively, which are comparable with the data reported in the literature. The adsorption mechanism of the concerned (radio)toxicants is proposed.