For this proof-of-concept host:guest assay and to validate that binding studies can be translated into a high-throughput automated protocol, the MOC (cage 1, Zn4(A1)4.(NTf2)8), concentration (0.0008 mmol/mL), host:guest ratio (1:4), and range of guests (32 neutral species), were selected based on literature precedents. For example, cage 1 has previously been reported to bind neutral guests such as t BuOH and cyclohexane, which were also included in the screen as controls to validate the workflow. The experiment concentration was selected where equimolar concentrations of the host and the host-guest complex would give a Ka ca. 10³ M⁻¹. This allows for stronger (Ka >> 10³ M⁻¹), intermediate (Ka ≃ 10³ M⁻¹) and weaker association (Ka << 10³ M⁻¹) to be estimated, based on previously reported ranges of values for Ka in related systems. Samples were prepared in 96-well plates using stock solutions on the Opentrons OT-2 (500 μL of 0.0008 M host in acetonitrile-d3 and 75 μL of 0.0214 M guest stock solutions in acetonitrile) before being sealed and vortexed at room temperature, and then transferred to high-throughput NMR tubes on the platform before being analyzed by 1 H NMR spectroscopy after 1 and 7 days (see Supporting Information Section S5 for full details). The accuracy of automated dispensing was also validated by checking the obtained host:guest ratio via integration of free cage 1 and unbound guest (Supporting Information Figure ), which confirmed a 1:4 stoichiometric ratio had been achieved.