Purely-organic clusterization‐triggered emission (CTE) has displayed promising abilities in bioimaging, chemical sensing, and multicolor luminescence. However, it remains absent in the field of circularly polarized luminescence (CPL) due to the difficulties in well-aligning the nonconventional luminogens. We report a case of CPL generated with CTE using the solid phase molecular self-assembly (SPMSA) of poly-L-lysine (PLL) and oleate ion (OL), that is, the macroscopic CPL supramolecular film self-assembled by the electrostatic complex of PLL/OL under mechanical pressure. Well-defined interface charge distribution, given by lamellar mesophases of OL ions, forces the PLL chains to fold regularly as a requirement of optimal electrostatic interactions. Further facilitated by hydrogen bonding, the through-space conjugation (TSC) of orderly aligned electron-rich O and N atoms leads to CTE-based CPL, which is capable of transferring energy to an acceptor via a Förster resonance energy transfer (FRET) process, making it possible to develop environmentally friendly and economic CPL from sustainable and renewable materials.

General strategies leading to scale-span molecular self-assembly are of crucial importance in creating bulk supramolecular materials. Here, we report that under mechanical pressure, caking of the precipitated molecular self-assemblies led to bulk supramolecular films. Massive fabrication of supramolecular films became possible by employing a simple household noodle machine. The film could be endowed to acquire diversified functions by depositing various functional ingredients via coprecipitation. We expect that our current work opens up a new paradigm leading to large-scale functional solid molecular self-assembled materials.

The brittleness of many supramolecular films in a dry environment has prevented their further application as supramolecular plastics. We report here the fabrication of supramolecular plastics displaying excellent dry-flexibility and mechanical strength through room-temperature solid-phase molecular self-assembly using water-locking polyelectrolyte and surfactant. Aided by mild mechanical pressure of about 0.5 MPa, the locked water enables the polyelectrolyte-bridged surfactant microdomains to merge into large mesophases to reduce the interface energy, which yields a transparent supramolecular film. The film still contains 2% water in a dry environment, which is capable of plasticizing the polyelectrolyte and surfactant; thus, it imparts excellent flexibility to the film. The dry film has a stress of 12 MPa and Young's modulus of 188 MPa with a strain of 24%. This mechanical strength is comparable to that of the commercial soft polyethylene plastics. Since the noncovalent interactions in the film can be activated by water under mild mechanical pressure within seconds, mending a broken film by pressing a wet patch with mild mechanical force onto the damage becomes possible. Complete recycling can be achieved under the same conditions. We envision the current roomtemperature mechanical force driven water-based recyclable and mendable supramolecular plastics would be very promising in reducing white pollution and generating integrated materials.