While only a small subset of variables was screened here under a single set of reaction conditions, the extensive structural diversity of reported MOCs has been achieved through variation of parameters that include the metal ion identity, the metal counterion, topicity of the ligand, the angle and spacing between the coordinating sites of a ligand, reaction stoichiometry, solvent choice, overall concentration, the reaction temperature, and sometimes the inclusion of a guest molecule to act as a template. This workflow could be readily extended to include reaction condition screening and template addition in the automated screening to further study the influence on the reaction outcome for conversion, reactivity and topological outcomes in the future. Pairing this automated experimental workflow with computational modelling allowed experimental observations to be rationalized post facto. Further work is needed to streamline the interconnection of these workflows to aid prediction in the future to direct synthesis. Finally, our automated workflow was extended to include screening of host-guest binding. A general knowledge of binding was readily achieved for a MOC, and trends elucidated, which in the future, may direct further studies and applications in molecular separations. In addition, while only a single solvent was used for the host-guest assay here, the workflow could be expanded to include different solvents, additional guests, a wider variety of MOCs, and different operational conditions. The dynamic nature of the assemblies, along with solvent and counterion effects, can drastically influence a MOC's ability to bind a guest. This limits our current ability to accurately predict binding through simulation, so screening this property in a highthroughput approach could be used to generate a host-guest binding database which can train predictive models for hostguest pairing with a high degree of accuracy.