Several methods for rapid sequestration, fluorometric detection, and the subsequent mass spectroscopic analysis of lanthanide ions using surface modified polystyrene magnetic microspheres are demonstrated. Mixed-ligand antenna complexes of Eu3+ in which one of the ligands is attached to the surface of the microspheres have been used as a means for the sequestration, immobilization, and detection of these ions. Using the ion-exchange properties of these microspheres, this scheme has been extended to the detection of nonluminescent ions. The principles of these assays form the basis for operation of a portable microfluidic device for general analytical and nuclear forensics applications and indicate the manner in which the established methods of analytical chemistry, such as liquid-liquid extraction and ion-exchange chromatography, can be adapted for such miniature devices.