A new class of biohybrid nanoprobes has been developed for surface-enhanced Raman scattering-based bioimaging. Silver nanoparticle clusters were encapsulated in polymeric nanoparticles using electrohydrodynamic jetting, followed by stabilization and bioconjugation. Controlled SERS intensity with high sensitivity, chemical stability, and biocompatibility makes the SERS biohybrid nanoprobes useful for bioimaging.