The use of heavy metals in technological applications has led to detrimental effects on human health and the environment. Activated carbon and ion-exchange resins are commonly used to remove pollutants but they are expensive. Therefore, the research of low-cost alternatives derived from natural resources and organic wastes is being considered. The aim of this study considers the use of Calcium Alginate/Spent Coffee Grounds (CA-SCGs) composite beads to adsorb heavy metals from aqueous solutions, particularly, the removal of Ni 2+ or Cd 2+ at concentrations from 10 ppm to 100 ppm. CA-SCGs beads were made of equal proportions of alginate and spent coffee grounds and compared with calcium alginate beads (CA beads) and spent coffee grounds (SCGs) in terms of capacity and rate of adsorption. Three cycles of adsorption/desorption were done. The beads were characterized by Scanning Electron Microscopy coupled with an energy-dispersive X-ray spectroscopy (SEM-EDX), Fourier-transform infrared spectroscopy (FT-IR), Raman spectroscopy, and point of zero charge. Langmuir, Freundlich, and Sips models, and a pseudo-second-order kinetic equation were used. Sips model showed the best correlation with the adsorption of CA-SCGs beads with capacities of adsorption of 91.18 mg/g for cadmium and 20.96 mg/g for nickel. CA-SCGs beads had a greater adsorption than the CA beads, achieving adsorption percentages close to 100% than alginate alone, showing their effectiveness in heavy metal removal.