The treatment of radioactive liquid waste containing organic compounds was always a cause for concern to radioactive waste management facilities because the processes available are expensive and difficult to manage. Biosorption has been studied as a new process in simulated wastes as an alternative to treating them. Among the potential biomass, the coconut fiber has very attractive features that allow the removal of radionuclides using a low-cost biosorbent. The aim of this study was to evaluate the capacity of coconut fiber to remove uranium, americium, and cesium from real radioactive liquid organic waste. Experiments with the biosorption of these radionuclides in coconut fiber were made including (1) preparation, activation, and characterization of biomass and (2) biosorption assays. The biomass was tested in raw and activated form. Biosorption assays were performed, adding the biomass to real waste solutions. The solutions contain natural uranium, americium-241, and cesium-137. The contact times and the concentrations range were varied. The radioisotopes remaining concentration in the solutions was determined by inductively coupled plasma optical emission spectrometry and gamma spectrometry. The results were evaluated by maximum experimental sorption capacity and isotherm and kinetics ternary models. The highest sorption capacity was observed with the activated coconut fiber, with values of 2 mg/g of U (total), 70E−06 mg/g of Am-241 and 40E−09 mg/g of Cs-137. These results suggest that biosorption with activated coconut fiber can be applied in the treatment of radioactive liquid organic wastes containing uranium, americium-241, and cesium-137.