Here, we describe an easy but robust chemical strategy to synthesize high-performance magnetic resonance (MR)/near-infrared (NIR) multimodal imaging nanoprobes. Poly(γ-glutamic acid) was used for the convenient phase transfer of MnFe(2)O(4) nanoparticles dispersed in organic solvents into aqueous solutions and facilitated further ionic gelation with poly(l-lysine). During the gelation process, MnFe(2)O(4) nanoparticulate satellites were encapsulated in the ionic nanocomplex, which induced synergistic magnetism and resulted in huge T(2) relaxivity (r(2)). The positively charged outer surfaces were assembled with other negatively charged NIR emitting fluorescent nanocrystals and enabled the highly efficient delivery of the magnetofluorescent polyelectrolyte nanocomposites (MagFL-PEN) into cancer cells. The enhancement of negative contrast of MagFL-PEN at 2 μg/mL concentration was similar to that of Resovist at 20 μg/mL concentration. The NIR fluorescence microscopy images of the MagFL-PEN-labeled cells even at 12.5 pM were able to be clearly observed. The labeling efficiency of MagFL-PEN was approximately 65-fold higher compared to that of the commercialized fluorescent nanocrystals, only after 3 h incubation period, even at the test concentration (100 pM). Due to the high-performance capabilities both in materials properties and cell labeling efficiency, the MagFL-PEN is expected to be used as a highly efficient MR/NIR dual-modality imaging nanoprobe in the detection of cancer cells and monitoring of therapeutic cells in vivo.