with the encapsulant being either solid elastic films [12][13][14][15][16] or solid-like jammed films of functional particles. [17][18][19][20][21] These films are rigid enough to stabilize nonequilibrium morphologies of the wrapped liquid, thus breaking the limit of equilibrium morphologies and further creating new shapes of wrapped, encapsulated fluids with inimitable functionalities.For traditional liquid-phase technologies, a liquid-like layer of surfactant or particles is usually used for wrapping and stabilizing liquid droplets. [22][23][24] Recent studies show that sufficiently thin elastic sheets offer a novel path to spontaneously wrap liquid droplets using capillary forces, where the elastic energy of curving sheets is balanced by the reduction of interfacial energy. [15,16,25,26] Although negligible at macroscopic scales, capillary forces become dominant and are able to bend the elastic sheets when the bending rigidity of elastic sheets is vanishingly small. [12,15,25] The robust elastic sheets allow the liquid drops to be trapped in nonequilibrium 3D shapes via a process that is usually referred to as capillary origami. [12,16,26] In previous wrapping studies, the final encapsulated 3D geometry was almost solely determined by the initial geometry of the flat thin elastic sheets, which made the process complicated and lacked versatility. The elastic sheets in previous reports were often conventional polymer thin films whose interfacial activities were too weak to manipulate the interfacial tension and participate in morphology evolution. [12,15,16] A large-scale elastic sheet [27] with a significant interfacial activity is desired to manipulate the interface that can adapt to various nonequilibrium shapes by external influence-a stimulant for evolved morphologies at the interface.Here, we report in situ formation of a large-scale surfactant sheet with strong interfacial activities by interfacial jamming of poorly soluble amphiphilic lignin macromolecules in particulate form at an oil/water interface. The amphiphilic nature of the surfactant sheet enables wrapping of either water or oil droplets, while its rigidity allows it to hold the liquid phases in various nonequilibrium morphologies. The surfactant sheet is physically networked by reversible hydrogen bonding and π-π interaction, which endows it with transforming and self-healing ability. The strong interfacial activity of the surfactant sheet results in an interfacial instability, which drives evolution of interfacial morphology and novel wrapped microstructures.Wrapping a 3D object with a 2D sheet is not uncommon, but the wrapping behavior becomes complex and interesting when the sheet is bestowed with strong interfacial activities. Amphiphilic lignin macromolecules, isolated from biomass, form a scalable thin surfactant sheet at an oil/water interface through the interfacial jamming process. The process marks three distinct stages of interfacial behavior: a) diffusive assembly, b) viscous assembly with retarded mobility, and c) flexible yet irre...