A Versatile Assembly Approach toward Multifunctional Supramolecular Poly(Ionic Liquid) Nanoporous Membranes in Water

Abstract Hydrogen (H)‐bonding‐integration of multiple ingredients into supramolecular polyelectrolyte nanoporous membranes in water, thereby achieving tailor‐made porous architectures, properties, and functionalities, remains one of the foremost challenges in materials chemistry due to the significantly opposing action of water molecules against H‐bonding. Herein, a strategy is described that allows direct fusing of the functional attributes of small additives into water‐involved hydrogen bonding assembled supramolecular poly(ionic liquid) (PIL) nanoporous membranes (SPILMs) under ambient conditions. It discloses that the pore size distributions and mechanical properties of SPILMs are rationally controlled by tuning the H‐bonding interactions between small additives and homo‐PIL. It demonstrates that, benefiting from the synergy of multiple noncovalent interactions, small dye additives/homo‐PIL solutions can be utilized as versatile inks for yielding colorful light emitting films with robust underwater adhesion strength, excellent stretchability, and flexibility on diverse substrates, including both hydrophilic and hydrophobic surfaces. This system provides a general platform for integrating the functional attributes of a diverse variety of additives into SPILMs to create multifunctional and programmable materials in water.