The ultimate success for a materials synthesis programme would be to first determine the structure we would like to make - with particular properties, such as shape-selective catalysis - which we would then predict how to make and then simply synthesise! As part of this effort, we are trying to both develop tools to aid with the synthesis design - through our template design efforts - and to develop an understanding of the self-assembly processes that occur during such syntheses. We employ a range of methods as appropriate - from ab initio modelling of key nucleation steps to forcefield-based Monte Carlo and de novo molecular assembly methods.