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Multimodal probes are an asset for simplified,improved medical imaging. In particular,fluorescence andmagnetic resonance imaging (MRI) are sought-after combinedcapabilities. Here, we show that pyrrolidin-2-one-capped man-ganese oxide nanoparticles (MnOpyrrNPs) combine MRI withfluorescence microscopy to function as efficient bifunctional bio-nanoprobes. We employ a one-pot synthesis forca.10 nm MnONPs, wherein manganese(II) 2,4-pentadionate is thermallydecomposed using pyrrolidin-2-one as a solvent and cappingligand. TheMnOpyrrNPs are soluble in water without any furtherpostsynthetic modifications. Ther1relaxivity andr2/r1ratioindicate that these NPs are potentialT1MRI contrast agents atclinical (3 T) and ultrahigh (9.4 T) magneticfields. Serendip-itously, the as-prepared NPs are photoluminescent. The unexpected luminescence is ascribed to the modification of thepyrrolidin-2-one during the thermal treatment.MnOpyrrNPs are successfully used to enablefluorescence microscopy of HeLacells, demonstrating bifunctional imaging capabilities. A low cytotoxic response in two distinct cell types (HeLa, HepG2)supports the suitability ofMnOpyrrNPs for biological imaging applications.