Resistance of pathogenic micro-organisms to conventional antibiotics is an essential issue for public health. The presence of such pharmaceuticals in aquatic ecosystems has been of major concern for which remediation and ultra-sensitive monitoring methods have been proposed. A less explored strategy involves the application of multifunctional nanosorbents for the uptake and subsequent detection of vestigial contaminants. In this study, colloidal nanoparticles (NPs) of iron oxide and gold were encapsulated in multi-layers of a charged polyelectrolyte (PEI: polyethyleneimine), envisaging the effective capture of tetracycline (TC) and its subsequent detection by Surface Enhanced Raman Scattering (SERS). Adsorption studies were performed by varying operational parameters, such as the solution pH and contact time, in order to evaluate the performance of the nanosorbents for the uptake of TC from water. While the magnetic nanosorbents with an external PEI layer (Fe3O4@PEI and Fe3O4@PEI-Au@PEI particles) have shown better uptake efficiency for TC, these materials showed less SERS sensitivity than the Fe3O4@PEI- Au nanosorbents, whose SERS sensitivity for TC in water has reached the limit of detection of 10 nM. Thus, this study highlights the potential of such magneto-plasmonic nanosorbents as multi-functional platforms for targeting specific contaminants in water, by taking into consideration both functionalities investigated: the removal by adsorption and the SERS detection across the nanosorbents' surfaces.