Ultrabright fluorescent nanoparticles (NPs) hold great promise for demanding bioimaging applications. Recently, extremely bright molecular crystals of cationic fluorophores were obtained by hierarchical coassembly with cyanostar anion-receptor complexes. These small-molecule ionic isolation lattices (SMILES) ensure spatial and electronic isolation to prohibit aggregation quenching of dyes. We report a simple, one-step supramolecular approach to formulate SMILES materials into NPs. Rhodamine-based SMILES NPs stabilized by glycol amphiphiles show high fluorescence quantum yield (30 %) and brightness per volume (5000 M  cm /nm ) with 400 dye molecules packed into 16-nm particles, corresponding to a particle absorption coefficient of 4×10  M  cm . UV excitation of the cyanostar component leads to higher brightness (>6000 M  cm / nm ) by energy transfer to rhodamine emitters. Coated NPs stain cells and are thus promising for bioimaging.

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http://dx.doi.org/10.1002/anie.202100950DOI Listing

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