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

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.