Diffusion of organic and inorganic molecules controls most industrial and biological processes that occur in a liquid phase. Although significant efforts have been devoted to the design and operation of large-scale purification systems, diffusion devices with adjustable biochemical characteristics have remained difficult to achieve. In this regard, micrometer-scale, bioinspired membranes with tunable diffusion properties have been engineered by covalent cross-linking of two elastin-like recombinamers (ELRs) at a liquid-liquid interface. The covalent approach selected provides the desired ELR-based membranes with structural support, and modulation of the concentration of the polypeptides employed confers direct control of the thickness, pore size, and diffusive properties over a broad range of molecular weights (4-150 kDa). The recombinant and versatile nature of the proteinaceous building blocks employed further paves the way to engineering bioactive motifs within the membrane scaffold, thereby widening their applicability in the biological field.