The vibrating-nozzle technology is very interesting to very easily and very rapidly produce industrial amounts of functional microspheres. The technology was used to make hybrid alginate silica microspheres by droplet coagulation. The microspheres were formed starting from suspensions of sodium alginate, and coagulation occurred in an aqueous solution of calcium ions. To enhance the mechanical properties of the alginate raw material, it was combined with two different silica sources: tetramethyl orthosilicate (TMOS) and commercial silica powder. The two different batches of alginate silica microspheres were fully compared with regard to their morphology, composition, shrinking behavior, and stability in acidic conditions. It was shown that the incorporation of an inorganic matrix resulted in a material with a better stabilized porous structure and a higher resistance in an acidic environment. Both are important when functional particles are designed to be used for adsorption of metal ions, either as a stirred suspension or as a stationary phase in a chromatographic column. A study of the adsorption performance was conducted in batch mode for neodymium(III), a representative element for the group of critical rare-earth elements. The effect of stripping (desorption) on the adsorption performance and reusability was also investigated. The functional alginate silica microspheres show a sustainable character.