Developing effective water treatment materials, particularly through proven adsorption methods, is crucial for removing heavy metal contaminants. This study synthesizes a cost-effective three-dimensional material encapsulating graphitic carbon nitride-layered double oxide (GCN-LDO) in sodium alginate (SA) through the freeze-drying method. The material is applied to remove uranium (U(VI)) and cadmium (Cd(II)) in real water systems. X-ray photoelectron spectroscopy (XPS) and Fourier transform infrared spectroscopy (FTIR) analyses conclusively verified the elemental composition and successful encapsulation of GCN-LDO within the SA matrix. Removal effectiveness was tested under various conditions, including adsorbent dose, ionic strength, contact time, temperature, different initial pollutant concentrations, and the impact of co-existing ions. The adsorption of U(VI) and Cd(II) conformed to the pseudo-second-order (PSO) kinetic model, signifying a chemical interaction between the sodium alginate-graphitic carbon nitride-layered double oxide (SA-GCN-LDO) sponge and the metal ions. The Langmuir isotherm indicated monolayer, homogeneous adsorption for U(VI) and Cd(II) with capacities of 158.25 and 165.00 mg/g. SA-GCN-LDO recyclability was found in up to seven adsorption cycles with a removal efficacy of 70%. The temperature effect study depicts the exothermic nature of the U(VI) and Cd(II) ion removal process. Various mechanisms involved in U(VI) and Cd(II) removal were proposed. Further, continuous fixed bed column studies were performed, and Thomas and the Yoon-Nelson model were studied. These insights from this investigation contribute to advancing our knowledge of the material's performance within the context of U(VI) and Cd(II) adsorption, paving the way for optimized and sustainable water treatment solutions.