This article studied the sorption behavior of Cs(I) ions from aqueous solutions onto molybdenum vanadate@bentonite (MoV@bentonite) composite. MoV@bentonite has been fabricated using the precipitation method and was characterized by different analytical tools including, FT-IR, XRD, and SEM attached with an EDX unit. The sorption studies applied on Cs(I) ions include the effect of contact time, pH, initial metal concentrations, ionic strength, desorption, and recycling. The experimental results revealed that in the adsorption process carried out after equilibrium time (300 min), saturation capacity has a value of 26.72 mg·g−1 and the sorption of Cs(I) ions is dependent on pH values and ionic strength. Sorption kinetic better fit with the pseudo-second-order model; sorption isotherms apply to Langmuir, Freundlich, and Dubinin-Radushkevich (D-R) isotherm models. Data of thermodynamic parameters indicate that sorption is spontaneous and endothermic. Recycling experiments show that MoV@bentonite could be used for 7 cycles and the best eluant for the recovery of Cs(I) ions is 0.1 M HCl (76.9%). All the obtained data clarify that MoV@bentonite is considered a promising sorbent for the sorption of Cs(I) ions from aqueous solutions.