Batch adsorption treatment using Iraqi bentonite as a natural adsorbent was adopted in this study to decontaminate actual 137Cs radioactive wastewater from the Al-Tuwaitha Nuclear Research Center, located south of Baghdad. The bentonite characterization was applied before and after treatment, using chemical compositions analyses, X-ray diffraction (XRD), scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDX), Brunauer–Emmett–Teller (BET) surface area analysis and Fourier-transform infrared spectroscopy (FT-IR). The batch adsorption mode was applied with the initial radioactivity concentration (1440.5 Bq/L), solid/liquid ratio (1 g/L), pH (6–8), contact time (1.5 h), and temperature (298°K). The adsorption experiments showed a decontamination removal efficiency of about 95.66% of 137Cs. A Freundlich adsorption isotherm model was approved for the adsorption of 137Cs, with a coefficient of determination R2 = 0.998. A pseudo-second-order model fitted well with the adsorption of 137Cs, with R2 = 0.983. The positive value of ΔH° in the thermodynamic results indicated that the adsorption process was endothermic physisorption (ΔH° = 15.01 kJ mol−1), spontaneous and favorable (ΔG° = −7.66 kJ mol−1 K−1), with a very low degree of disorder (ΔS° = 0.076 kJ mol−1 K−1).