Fibroblast‐Mimetic Lignin Polymersomes for Logic‐Gated Synthesis of Mechanically Reconfigurable Bioskins

ABSTRACT Ageing is inevitable and accompanied by progressive loss of skin elasticity. Fibroblasts, embedded within the extracellular matrix, finely regulate skin mechanics via membrane‐bound ligands. Creating synthetic assemblies that mimic fibroblast function is appealing yet challenging. Here, we present a strategy that co‐assembles lignin with divinyl ligands to generate fibroblast‐mimicking polymersomes, enabling precise programming of bulk materials to emulate human skin across distinct physiological stages. Because lignin polymersomes are driven by relatively weak π–π stacking, hydrophobic ligands efficiently intercalate among aromatic rings, and their interfacial distribution can be tuned via molecular engineering. The polymersomes can be programmed in a Boolean logic‑gate manner (OR, AND, and NOT) to synthesize skin‐mimetic gels with tailored mechanical properties, analogous to fibroblast behavior. Furthermore, the platform enables on‑demand, high‑resolution 3D printing of complex bioskin architectures. This work provides a biomimetic paradigm for the synthesis and precise control over assembly from the molecular to the macroscopic scale.