Single Molecular Layer of Chitin Sub‐Nanometric Nanoribbons: One‐Pot Self‐Exfoliation and Crystalline Assembly into Robust, Sustainable, and Moldable Structural Materials

Sub‐nanometric materials (SNMs) represent a series of unprecedented size‐/morphology‐related properties applicable in theoretical research and diverse cutting‐edge applications. However, in‐depth investigation and wide utilization of organic SNMs are frequently hindered, owing to the complex synthesis procedures, insufficient colloidal stability, poor processability, and high cost. In this work, a low‐cost, energy‐efficient, convenient, effective, and scalable method is demonstrated for directly exfoliating chitin SNMs from their natural sources through a one‐pot “tandem molecular intercalation” process. The resultant solution‐like sample, which exhibits ribbon‐like feature and contains more than 85% of the single molecular layer (thickness 85% of single molecular layer. Thanks to the sub‐nanometric size and rich surface functional groups, these nanoribbons reveal versatile intriguing properties that rarely observed in their nano‐counterparts (nanofibrils), and thus provide new platform for both theoretical study and practical applications of organic sub‐nanometric materials.