Hierarchically ordered planar and spherical membranes (sacs) were constructed using amphiphilic and cationic β-sheet peptides that spontaneously assembled together with negatively charged alginate solution. The system was found to form either a fully developed membrane structure with three distinct regions including characteristic perpendicular fibers or a non-fully developed contact layer lacking these standing fibers, depending on the peptide age, membrane geometry and membrane incubation time. The morphological differences were found to strongly depend on fairly-long incubation time frames that influenced both the peptide's intrinsic alignment and the reaction-diffusion process taking place at the interface. A three-stage mechanism was suggested and key parameters affecting the development process were identified. Stability tests in biologically relevant buffers confirmed the suitability of these membranes for bio applications.
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