Graphite (GR) and graphite/alginate (GRA) composite were synthesized utilizing the thermal annealing technique and used as a new adsorbent material for the selective separation and removal of La(III) and Ce(III) from aqueous solutions. Fourier transform infrared (FTIR) spectroscopy, thermal analysis (DTA, TGA), X-ray diffraction (XRD), surface area, porosity, and scanning electron microscope (SEM) were also used to characterize the generated material. Distinct experiments were performed to test the ability of the GRA to La(III) and Ce(III) removal, which include the effect of pH, shaken time, initial concentration of La(III), and Ce(III) at different temperatures range. After 20 min, both ions have reached equilibrium. The pseudo second-order kinetic model was chosen as one which best fits the experimental evidence and better reflects the chemical sorption process. Adsorption isotherm was studied using the Langmuir, Freundlich, and D-R models. The Langmuir model was used to better fit the results obtained. At 25 °C, Ce(III) and La(III) have maximum monolayer capacities of 200 and 83.3 mg/g, respectively. The sorption was endothermic reaction and spontaneous, as illustrated by the data of thermodynamics studies. GRA has the ability to be used as a novel lanthanide adsorbent material, especially for selective separation between Ce(III) and La(III).