Small‐Molecule‐based Supramolecular Plastics Mediated by Liquid‐Liquid Phase Separation**

Plastics are one of the most widely used polymeric materials. However, they often undegradable and non-recyclable due to very stable covalent bonds macromolecules, causing environmental pollution health problems. Here, we report that liquid-liquid phase separation (LLPS) could drive formation robust, stable, sustainable plastics using small molecules. The LLPS process sequester concentrate solutes, strengthen non-covalent association between molecules produce a bulk material whose property was highly related encapsulated water amounts. It robust plastic with remarkable Young's modulus 139.5 MPa when content low while became adhesive instantly self-heal more absorbed water. Finally, responsiveness enabled be recyclable. This work allowed us understand at molecular level demonstrated is promising approach exploring eco-friendly supramolecular potential substitutes for conventional polymers.