Biomolecular 1D Necklace-like Nanostructures Tailoring 2D Janus Interfaces for Controllable 3D Enteric Biomaterials

Construction of well-ordered two-dimensional (2D) and three-dimensional (3D) assemblies using one-dimensional (1D) units is a hallmark of many biointerfaces such as skin. Mimicking the art of difunctional properties of biointerfaces, which skin exhibits as defense and shelter materials, has inspired the development of smart and responsive biomimetic interfaces. However, programming the long-range ordering of 1D base materials toward vigorous control over 2D and 3D hierarchical structures and material properties remains a daunting challenge. In this study, we put forward construction of 3D enteric biomaterials with a two-strata 2D Janus interface assembled from self-adaptation of 1D protein–polysaccharide nanostructures at an oil–water interface. The biomaterials feature a protein dermis accommodating oil droplets as a reservoir for bioactive compounds and a polysaccharide epidermis protecting them from gastric degradation. Furthermore, the epidermis can be fine-tuned with different thicknesses rendering enteric delivery of a bioactive cargo (coumarin-6) with controllable retention in the intestinal tract from 6 to 24 h. The results highlight a skin-inspired construction of enteric biomaterials by self-adaptation of 1D nanostructures at the oil–water interface toward 2D Janus biointerfaces and 3D microdevices, which can be tailored for intestinal treatments with intentional therapeutic efficacies.