A promising graphene polymeric composite was synthesized using gamma irradiation of reduced graphene oxide (RGO); itaconic acid (IA) grafted starch (St) and 16, 16-dimethylheptadecan-1-amine (PJMT). The prepared composite (HGPC) and RGO were characterized using different analytical methods such as FT-IR, SEM, DTA-TGA, XRD, particle size distribution, and pore size distribution. Then after, they were assessed as sorbents for removal of europium radionuclides from aqueous solutions at pH 3, volume-to-mass ratio 0.1 L g−1 and 25 °C. The sorption reaction reached the equilibrium after 4 h. The Qmax attained the values of 106.79 and 11.46 mg g−1 for Eu(III) sorption onto HGPC and RGO, respectively. The values of the isotherm parameters confirmed that a chemisorption mechanism controlled the sorption process. The calculated thermodynamic parameters demonstrated that the sorption of Eu(III) by HGPC was a spontaneous and endothermic process. 83.53% and 84.09% of europium radionuclides were effectively eluted from loaded materials using 0.1 M EDTA and 0.1 M HCl solutions, respectively.