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Layered materials are desirable targets in designing crystalline architectures, due to their many distinct, favourable physical properties. For example, in the pharmaceutical manufacturing industry, layered materials are more compactable into tablets, especially where the interactions between layers are much weaker than those within the layers, while in the design of porous materials, layered materials are much more likely to lead to channel structures and therefore provide an easy route to solvent or gas exchange. Crystal engineering is a welldeveloped approach for generating supramolecular constructs, mainly using hydrogen bonding as its structure-directing tool. However, it is often the presence of weaker interactions which lead to the formation of a truly layered structure this is inevitably more difficult to control and can also often lead to the presence of significant structural defects, some of them beneficial to function. We have developed a wide range of approaches for generating layered materials from multi-component crystallisations. This has not only involved conventional co-crystallisation of more than one molecule into the crystalline lattice, but also utilising co-molecules in a templating role, guiding the assembly of molecules towards a layered crystalline form. Amongst the significant findings in engineering and controlling the assembly of materials whose functionality is based on a layered architecture, the following will be discussed: • a simple and reliable route to the formation of paracetamol Form II, a layered metastable polymorph with favourable compaction properties, produced through templating multi-component crystallisation [1]; • the porous, layered molecular material 4-phenoxyphenol, which is based on a dominant hexagonal hydrogen bonded motif, with breathable channels that are robust when both solvent-filled and empty; • layered, channel-containing molecular complexes of nucleic acid bases, that show promise for the possibility of solvent or gas exchange, where C-H∙∙∙F hydrogen bonds are integral to the formation of channels; • multi-component systems including hydrates of both phloroglucinol and gallic acid in which solvent molecules play a crucial role in constructing and connecting the layers, and whose disposition can be elucidated by a combination of diffraction and quantum chemical calculations. The significant functional features of these structures are both layered and porous channel architectures, and the locally ordered defect structure is also vital to their function. These functional molecular materials have as a common theme, a strongly hydrogen bonded motif, assembled into layers by weaker or stronger interlayer interactions, together with the possibility of local ordering, all of which can be vital in lending these materials their particular potential functional capabilities. [1] L.H. Thomas, C. Wales, L. Zhao, and C.C. Wilson, Cryst. Growth Des. 2011. [2] L.H Thomas, G.A. Craig, C.A. Morrison, A.M. Reilly and C.C. Wilson, Cryst. Growth Des. 2011.

Structural diversity in layered organic materials through templating co-crystallisation