| Summary: | This thesis describes the design and characterisation of self-assembled systems that employ Coulombic interactions as the primary means for driving assembly. Hierarchical self-assembly is sought in three different areas: mesoporous materials, two-dimensional polymers, and peptide fibres. Chapter 1 presents a general introduction to the rationale for using self-assembly to achieve nanotechnology, the basic principles of self-assembly, and an introduction to charge-based assembly, mesoporous materials, two dimensional polymers, and peptide fibres. Chapter 2 describes a new method to synthesise mesoporous membranes, which may contain silica, using ionic self-assembly. These materials result from combining polyelectrolytes with surfactants and inorganic precursors at liquid-liquid interfaces to give a columnar structure perpendicular to their surface. Chapter 3 describes the theoretical design requirements for a tecton that assembles to form a two-dimensional self-assembled polymer. Based on these rules a peptide-based building block is designed, synthesised, and characterised along with the resulting two-dimensional sheets. Chapter 4 continues the topic of 20 polymers with two next-generation systems for studying the assembly of two-dimensional peptide sheets. Chapter 5 describes research towards achieving hierarchical assembly with Self-Assembled Peptide Fibres using layer-by-layer self-assembly and electrophoretic deposition
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