Aromatic donor modified prolinamide and aromatic acceptor modified thiourea were synthesized. They self‐assembled into a cooperative organocatalytic system through the aromatic donor‐acceptor interaction and catalyzed aldol reactions in high yields and stereoselectivity on water. The aromatic donor‐acceptor interaction was confirmed by mass spectrum, UV‐vis titraition and 1H‐NMR titration experiments.
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