A grand challenge in science is the controlled assembly of atoms and molecules into novel forms as the basis for new physical phenomena and next-generation technologies. This programme will focus on excellence in synthesis of advanced inorganic functional materials through the development of fundamental capabilities for control of structure and composition in crystalline materials with large unit cells that are resilient to the introduction of multiple functionality. The targeted synthesis of these materials is addressed by developing a smart intuition approach in which detailed chemical appreciation of the structure-composition-property relationships is focused by predictive computation. The task is structured as a computation and growth-led Theme 1, where nanodeposition tools and tightly controlled sub-structure selection focus the computational task, and a synthesis- and measurement lead Theme 2 where compositional and structural features controlling complex properties are identified to initially define target materials selection. Theme 1 initially addresses the assembly of modular thin film and bulk materials to permit the required methodology development. Theme 2 will identify a toolkit of chemical components by synthesis and measurement (encompassing both average and local structure and dynamics) that will then be analysed predictively by computation to identify specific compositions for synthesis. The developed capability will integrate computation as a focused tool in the synthesis of complex materials, rather than devising an approach capable of surveying all possible compositions. It will permit the isolation of specific structures within a focused space of components, identified by structure-property-composition analysis in bulk materials (specifically those where structural frustration is imposed by competing interactions between multiple sublattices) or by selection of modules for unit cell by unit cell assembly of thin films.