There are many great uses for heavy elements that are expanding daily and generating enormous amounts of effluents. Therefore, tremendous scientific efforts in removing, recovering, and recycling them are carried out to prevent these harmful effects on the environment and human health. The polyacrylic-carboxymethyl cellulose-trioctyl amine/reduced graphene oxide adsorbent (AA-CMC-TOA/rGO) was synthesized as a promising sorbent for Zr4+ and Y3+ ions by gamma irradiation for a mixture of acrylic acid, carboxymethyl cellulose, and trioctyl amine as an organic solvent. A complete characterization of the manufactured composite was carried out to find out its chemical and physical properties several techniques such as XRD, EDX, SEM, FT-IR, TGA-DTA, and BET. Several factors affecting the Zr4+ and Y3+ adsorption processes were studied to set the best conditions that achieve the extreme loading capacity of Zr4+ and Y3+ ions. Loading capacities of 0.99 and 1.07 mmol g−1 were achieved for Zr4+ and Y3+, respectively. The results of the kinetic models indicated that the adsorption reactions of Zr4+ and Y3+ ions were carried out via a chemical reaction mechanism. Langmuir, Dubinin–Radushkevich, and Redlich–Peterson models accurately described the adsorption isotherm data by proving their chemical nature. The results of thermodynamics added evidence of the chemical nature, spontaneous, and endothermic nature of the adsorption processes. A complete retrieval for Zr4+ and Y3+ ions contents located in the effluent was efficiently achieved using AA-CMC-TOA/rGO sorbent which proved its uses as a promising sorbent.