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Organic self‐assembled co‐crystals have garnered considerable attention due to their facile synthesis and intriguing properties, but supramolecular interactions restrict their stability in aqueous solution, which is especially important for biological applications. Herein, we report on the first biological application of aqueous dispersible self‐assembled organic co‐crystals via the construction of metal–organic framework (MOF) ‐stabilized co‐crystals. In particular, we built an electron‐deficient MOF with naphthalene diimide (NDI) as the ligand and biocompatible Ca2+ as the metal nodes. An electron donor molecule, pyrene, was encapsulated to form the host–guest MOF self‐assembled co‐crystal. We observed that such MOF structure leads to uniquely high‐density ordered arrangement and the close intermolecular distance (3.47 Å) of the charge transfer pairs. Hence, the concomitant superior charge transfer interaction between pyrene/NDI can be attained and the resultant photothermal conversion efficiency of Py@Ca‐NDI in aqueous solution can thus reach up to 41.8 %, which, to the best of our knowledge, is the highest value among the reported organic co‐crystal materials; it is also much higher than that of the FDA approved photothermal agent ICG as well as most of the reported MOFs. Based on this realization, as a proof of concept, we demonstrated that such a self‐assembled organic co‐crystal platform can be used in biological applications that are exemplified via highly effective long wavelength light photothermal therapy. [ABSTRACT FROM AUTHOR]

Keywords: charge-transfer interaction; metal-organic framework; organic co-crystal; photothermal therapy; self-assembly EN charge-transfer interaction metal-organic framework organic co-crystal photothermal therapy self-assembly 23465 23465 1 10/20/21 20211025 NES 211025 B Lanterns on water b resemble aqueous dispersible metal-organic framework (MOF) structures composed of an alternating arrangement of donor and acceptor molecules. GLO:44U/25oct21:anie202111740-toc-0001.jpg PHOTO (COLOR): . gl GLO:44U/25oct21:anie202111740-toc-0001.jpg PHOTO (COLOR): . gl B Lanterns on water b resemble aqueous dispersible metal-organic framework (MOF) structures composed of an alternating arrangement of donor and acceptor molecules. Charge-transfer interaction, metal-organic framework, organic co-crystal, photothermal therapy, self-assembly. [Extracted from the article]

Charge-transfer interaction, metal-organic framework, organic co-crystal, photothermal therapy, self-assembly Keywords: charge-transfer interaction; metal-organic framework; organic co-crystal; photothermal therapy; self-assembly EN charge-transfer interaction metal-organic framework organic co-crystal photothermal therapy self-assembly 23657 23657 1 10/20/21 20211025 NES 211025 B Lampions auf dem Wasser b repräsentieren in Wasser dispergierbare metallorganische Gerüststrukturen (MOFs), die aus einer alternierenden Anordnung von Donor- und Akzeptormolekülen bestehen. Titelbild: Self-Assembled Metal-Organic Framework Stabilized Organic Cocrystals for Biological Phototherapy (Angew. [Extracted from the article]